This thesis presents a novel micron-sized trapezoidal plasmonic waveguide design, called an Interface Plasmon Polariton waveguide. The guiding mechanism is explained using an effective index method and validated by simulations. The mode cut-off conditions and single-mode guiding properties are both determined using simulation and experimentally demonstrated. The waveguides have a long 1 mm propagation distance at 1550 nm wavelengths. Using this IPP waveguide, novel dielectric rib, dielectric varying-density hole-array, and metal-groove Bragg grating $\emph{in vitro}$ sensors are designed, fabricated, and characterized. The devices have a 1100 nm/RIU sensitivity and 0.006 RIU sensing resolution obtained from measurements and are validated by theory. The IPP sensors developed in this thesis not only offer competitive plasmonic sensitivity, sensing resolution, signal to noise ratio, result reproducibility, and reusability, they are also easy to fabricate and simple to package. Therefore, these new sensor designs are an enabler for lab-on-a-chip platforms to adapt plasmonic technology.

In this thesis numerical methods are used to understand the individual and collective optical response of metal nanoparticles (MNPs). In particular, finite 1D assemblies of MNPs are characterized by analytical solutions to Maxwell's equations. Small particle solutions such as the well-established plasmon hybridization scheme as well as a novel circuit model explaining the intrinsic mechanisms of free electron dynamics help to characterize the optical response of single and coupled MNPs. Complex systems of closely spaced MNPs with small interparticle gaps are studied with the help of full scattering solutions to Maxwell's equations. It is shown that higher order plasmon modes facilitate strong near-fields between MNPs, and in linear chains foster specific optical attributes which are present in more complex systems, playing a key role in energy propagation along practical MNP waveguides.

Recent scientific progress has resulted in the development of sophisticated hybrid nanostructures composed of semiconductor and metal nanoparticles. These hybrid structures promise to produce a new generation of nanoscale optoelectronic devices that combine the best attributes of each component material. The optical response of metal nanostructures is dominated by surface plasmon resonances which create large local electromagnetic field enhancements. When coupled to surrounding semiconductor components, the enhanced local fields result in strong absorption/emission, optical gain, and nonlinear effects. Although hybrid nanostructures are poised to be utilized in a variety of applications, serious hurdles for the design of new devices remain. These difficulties largely result from a poor understanding of how the structural components interact at the nanoscale. The interactions strongly depend on the exact composition and geometry of the structure, and therefore, a quantitative comparison between theory and experiment is often difficult to achieve. Colloidal semiconductor quantum dots are strong candidates for integration with metal nanostructures because they have a variety of desirable optical properties, such as tunable emission and long term photostability. However, one potential drawback of colloidal quantum dots is the intermittency in their fluorescence (commonly referred to as “blinking”). Blinking was first observed over a decade ago, yet there is still no complete theory to explain why it occurs. In spite of the lack of a full theoretical explanation, multiple methods have been used to reduce blinking behavior, including modifying quantum dot interfaces and coupling quantum dots with metal nanostructures. This thesis focuses on studying the coupling between colloidal quantum dots and metal nanoparticles in simple model systems. Atomic force microscopy nanomanipulation is used to assemble the hybrid structures with a controlled geometry. The experimental studies report for the first time the modified fluorescence decay, emission intensity, and blinking of a single quantum dot coupled to a single Au nanoparticle. Since the geometry of the structure is known, these studies provide reliable information on the interparticle coupling, and quantitative experimental results are shown to be consistent with classical electrodynamic theories. / text

We present a novel concept to design apertureless plasmonic probes for near-field scanning optical microscopy (NSOM) with enhanced optical power throughput and near-field confinement. Specifically, we combine unidirectional surface plasmon polariton (SPP) generation along the tip lateral walls with nanofocusing of SPPs through adiabatic propagation towards an apertureless tip. Three probe designs are introduced with different light coupling mechanisms. Optimal design parameters are obtained with 2D analysis and realistic probe geometries with patterned plasmonic surfaces are proposed using the optimized designs. The electromagnetic properties of the designed probes are characterized in the near-field and compared to those of a conventional single-aperture probe with same pyramidal shape. The optimized probes feature enhanced light localization in near-field of tip apex and improved optical throughput. Our ideas effectively combine the resolution of apertureless probes with throughput levels much larger than those available even in aperture-based devices. / text

The optical and magneto-optical response of plasmonic resonances in metallic nanoarrays out of square structures, either in holes or islands, were investigated. The excitation of the Bragg Plasmons takes place within a grating. Significant differences in the excited plasmon modes were seen by using p- or s-polarized light as well between the holes and islands sample. In order to investigate magneto-optical response from the magnetic nanostrucures, transverse magneto-optical Kerr effect (TMOKE) measurements were done with the result that there is a difference in holes and islands sample. Contrary to what is generally expected for the polarization dependence of TMOKE, a TMOKE signal for s-polarized light on the holes sample was measured.

This thesis presents optofluidic nanostructures for analyte transport, concentration and sensing. This work was part of a larger collaborative project between the BC Cancer Agency and the departments of Chemistry, Electrical and Mechanical Engineering at the University of Victoria. In this work, arrays of nanoholes are used as optofluidic platforms for sensing, combining the characteristics of these nanostructures for both fluidic transport and plasmonic (optical) sensing. Two different modes are considered: flow-over mode, where the sample solution containing the analyte flows on top of the nanohole arrays, and a novel flow-through mode, where the nanoholes are used as nanochannels, enabling solution transport and analyte sieving. Flow-through nanohole array operation and sensing is first demonstrated, offering a six-fold improvement in sensor response compared to established flow-over sensing formats. Through a subsequent theoretical scaling analysis and computational analyses, the benefits of the flow-through nanohole sensing format are further quantified. A first analysis is dedicated to study the enhancement offered by the flow-through operation mode using a mass transport approach. A second analysis offers an ample study of benefits and limitations of the flow-through nanostructure operation using the combination of mass transport and binding kinetic parameters for different analytes with characteristics of clinical relevance. The mass transport analysis indicates much higher analyte collection efficiency (~ 99%) offered by the flow-through mode, compared to the flow-over platform (~ 2%). The analysis including both mass transport and binding kinetics demonstrate up to 20-fold improvement in response time for typical biomarkers. This thesis also presents the use of the flow-through optofluidic platform as an active analyte concentrator. In combination with a pressure bias, an electric field is used to concentrate electrically charged analyte for subsequent sensing. Fluorescein enrichment of 180-fold in 60 s was achieved, and 100-fold enrichment and simultaneous surface plasmon resonance (SPR) sensing of a protein (bovine serum albumin, BSA) was demonstrated. These experiments represent the first active utilization of a nanohole metallic layer as an electrode, and the first demonstration of a photonic nanostructure achieving both concentration and sensing of analytes. Towards the integration of optofluidic nanostructures into microfluidic environments for portable lab-on-chip diagnostic systems, this dissertation also includes the development of two nanohole array based sensing systems with simple flow-over operation. The first system consisted of a hand-held device with a dual-wavelength light source to increase the spectral diversity. The second system consisted of nanohole arrays integrated with a microfluidic concentration gradient generator for the detection and quantification of ovarian cancer antibody and antigen. Additionally, this dissertation includes a novel technique to actuate liquids in microchannels through ground-directed electric discharges. Experiments demonstrate average fluid velocities on the order of 5cm/s and applicability of the technique in serpentine channels, for on-demand fluid routing, to initiate a mixing process, and through an on-chip integrated microelectrode. / Graduate

Metal nanostructures, with their extraordinary optical properties, have attracted great attention in recent years. Subwavelength-scaled metal elements, without involving array effects, have the unique ability to confine or route light at the nano-scale. In this thesis, we provide three topics relating to the manipulation of light using metal nanostructures. We first present a theory to solve the end-face reflection of a subwavelength metal stripe, which is beneficial to the design of optical resonator antennas. Subsequently, we take the advantage of the destructive interference among triple nano-slits to sharpen the focus beam in the near-field at near-infrared wavelengths, which is of interest to the study of near-field optical phase imaging and lithography. Lastly, we demonstrate a rectangular subwavelength aperture quad to convert linearly polarized radiation to a radially polarized beam, which is useful to create a deep-subwavelength focus and for optical trapping. / Graduate

This dissertation contains analytical and numerical studies of nonlinear surface-plasmon polaritons (SPPs). In our studies, we consider SPP propagation at the interface between a noble metal with a cubic optical nonlinearity and an optically linear dielectric. We first consider a sum-frequency generation process during the nonlinear interaction, where a nonlinear polarization with tripled frequency is generated from the incident fundamental SPP. Using the non-depletion approximation, the solution of the nonlinear wave equation shows a third harmonic generation process from the incident SPP wave. The solution is bound in the dielectric while freely propagating in the metal. For realistic noble metals with absorption, we use silver for its transparency window around the plasma frequency. In this window, absorption losses are reduced and the resultant signal has a good transmittance within the metal. The energy conversion efficiency from the incident SPP wave to the THG signal is about 0.1% for excitation using a standard continuous wave laser with visible light intensity I = 103W/cm2. Once generated, the propagation angle of the signal is fully determined by the optical properties of the dielectric and the metal layers. We next consider a nonlinear polarization with the same frequency as the incident light. In this process the third order nonlinearity of the metal is described by a nonlinear optical refractive-index. With the slowly varying amplitude approximation, the nonlinear wave equation takes the form of a nonlinear temporal Schr¨odinger (NLS) equation. The solution to the NLS equation for the nonlinear SPP is a temporal dark soliton (TDS). In addition to analytical studies, computational methods are also used. With no metal loss, the numerical solution shows stable propagation of a TDS, when the initial pulse has a tanh envelope satisfying the threshold peak amplitude. For an arbitrary input pulse, instabilities such as background-oscillations and multi-peak breakups occur. With metal loss, the input optical pulse decays while maintaining a single pulse shape when the initial amplitude satisfies the same tanh envelope condition as in the lossless case. For an arbitrary pulse, background-oscillations or pulse-breakups occur after a short time of propagation.

Nanometallic structures efficiently convert light to surface plasmon-polaritons (SPPs) localized to ultra-small volumes. Such structures can provide highly enhanced fields and are of interest in applications involving plasmon-enhanced nonlinear optics. In this study, the devices consist of rectangular gold nanoantennas on a graphene layer on a SiO2/Si substrate. The nanoantennas are used to exploit SPPs to enhance the interaction between graphene and light. Specifically, plasmon-enhanced Raman scattering from graphene is of interest. Here, the nanoantennas are spectrally-aligned with a Stokes wavelength of graphene. With the addition of a second laser source, stimulated Raman scattering can be achieved. The first laser source pumps the sample’s atoms and molecules into virtual excited states and the second one stimulates emission of a photon and relaxation to a higher mode of the ground state. This work involves designing and constructing a stimulated and spontaneous Raman microscope and also a reflectance measurement tool. Within the framework of this thesis, Raman scattering enhancement in graphene based on plasmonic resonant enhancement of the Stokes emission is demonstrated, providing a maximum cross-sectional gain of approximately 500 per antenna. This work also shows the normalized reflectance response of the nanoantenna structures of different length and width and how their resonant wavelengths shift.

This thesis contributes to the realisation of plasmonic lasers based on plasmon polariton Bragg gratings. The scope of this thesis is twofold. In the first section, entitled Passive plasmonic Bragg grating characterization, the results of the testing and characterization of a new design of plasmonic Bragg gratings in the near-infrared are presented. The reflection and transmission responses expected from plasmon-polariton Bragg gratings (PPBGs) are treated theoretically using the transfer matrix method (TMM) and the numerical model is validated experimentally. The experimental setup and procedures are then described in detail. Results show that the near-infrared plasmon polariton Bragg gratings possess a Bragg reflection at a wavelength close to the Bragg wavelength predicted by TMM. In the second section, Gain optimisation and bleaching of IR-140 doped PMMA, an in-depth analysis of the gain medium (IR-140 dye doped poly(methyl methacrylate) better known as PMMA) is performed. This gain medium was selected as a gain layer for active plasmonic gratings and distributed feedback lasers designed by a colleague Ph.D. candidate. The optimized molecular weight of IR-140 in PMMA was found to be 0.9% to obtain a material gain of 81 cm-1.