The problem of heavy material and radiative losses in plasmonic devices has held back their implementation for compact and high-speed data storage and interconnects. One of the most interesting solutions to this problem currently under exploration is the addition of a gain material in close proximity to the metallic nanostructures for loss compensation. Here the physics of light transport in a nanoparticle array, and the operation of gain media in contact with the structure, are described and analytically modeled. A two-dimensional array of closely spaced gold nanoparticles has been fabricated by focused ion beam milling, and its electromagnetic response in the presence or absence of a dye coating has been simulated in preparation for pump-probe optical testing. The compensation of losses via a fluorophore coating has been proven for the first time in this geometry, for a physically realized sample. / text

This thesis details original experimental investigations in to the interaction of light with the mobile electrons at the surface of metallic diffraction gratings. The gratings used in this work to support the resultant trapped surface waves (surface plasmon polaritons), may be divided into two classes: ‘crossed’ bigratings and ‘zigzag’ gratings. Crossed bigratings are composed of two diffraction gratings formed of periodic grooves in a metal surface, which are crossed at an angle relative to one another. While crossed bigratings have been studied previously, this work focuses on symmetries which have received comparatively little attention in the literature. The gratings explored in this work possesses two different underlying Bravais lattices: rectangular and oblique. Control over the surface plasmon polariton (SPP) dispersion on a rectangular bigrating is demonstrated by the deepening of one of the two constituent gratings. The resulting change in the diffraction efficiency of the surface waves leads to large SPP band-gaps in one direction across the grating, leaving the SPP propagation in the orthogonal direction largely unperturbed. This provides a mechanism to design surfaces that support highly anisotropic propagation of SPPs. SPPs on the oblique grating are found to mediate polarisation conversion of the incident light field. Additionally, the SPP band-gaps that form on such a surface are shown to not necessarily occur at the Brillouin Zone boundaries of this lattice, as the BZ boundary for an oblique lattice is not a continuous contour of high-symmetry points. The second class of diffraction grating investigated in this thesis is the new zigzag grating geometry. This grating is formed of sub-wavelength (non-diffracting) grooves that are ‘zigzagged’ along their length to provide a diffractive periodicity for visible frequency radiation. The excitation and propagation of SPPs on such gratings is investigated and found to be highly polarisation selective. The first type of zigzag grating investigated possesses a single mirror plane. SPP excitation to found to be dependant on which diffracted order of SPP is under polarised illumination. The formation of SPP band-gaps is also investigated, finding that the band-gap at the first Brillouin Zone boundary is forbidden by the grating’s symmetry. The final grating considered is a zigzag grating which possesses no mirror symmetry. Using this grating, it is demonstrated that any polarisation of incident light may resonantly drive the same SPP modes. SPP propagation on this grating is found to be forbidden in all directions for a range of frequencies, forming a full SPP band-gap.

The modification of spontaneous emission, i.e. the Purcell effect, with optical cavities has been highly studied over the past 20 years as one of the most important goals for cavity quantum electrodynamics (cQED). The recent development of using surface plasmon resonances to concentrate optical field into sub-wavelength scale further extended cQED research of into a new regime. However, although metallic reflectors are used in some of the earliest demonstrations of cQED, the use of metals is not preferable in high Q optical cavities due to the lossy nature of metals. The presence of metals near an optical emitter also strongly alters its radiation dynamics. As a result, the development of plasmonic cavities brings not only new opportunities but also new problems and challenges. In this thesis we describe four different plasmonic cavity designs along with optical simulations and measurements on them to demonstrate: large spontaneous emission enhancement, controlled mode tuning, and control of the plasmonic band-gap and resonances of high-Q plasmonic cavities for coupling to specific emitters. We hope that our work can guide and inspire researchers who are moving from traditional cavity designs to novel plasmonic devices, helping them to establish design concepts, fabrication criteria, and baselines for characterizing these devices. / Engineering and Applied Sciences

The coupling of macroscopic objects via the optical near-field can generate strong attractive and repulsive forces. Here, I explore the static and dynamic optomechanical interactions that take place in a geometry consisting of a silicon nanomembrane patterned with a square-lattice photonic crystal suspended above a silicon-on-insulator substrate. This geometry supports a hybridized optical mode formed by the coupling of eigenmodes of the membrane and the silicon substrate layer. This system is capable of generating nanometer-scale deflections at low optical powers for membrane-substrate gaps of less than 200 nm due to the presence of an optical cavity created by the photonic crystal that enhances both the optical force and a force that arises from photo-thermal-mechanical properties of the system. Feedback between Brownian motion of the membrane and the optical and photo-thermal forces lead to dynamic interactions that perturb the mechanical frequency and linewidth in a process known as ``back-action.'' The static and dynamic properties of this system are responsible for optical bistability, mechanical cooling and regenerative oscillations under different initial conditions. Furthermore, solid objects separated by a small distance experience the Casimir force, which results from quantum fluctuations of the electromagnetic field (i.e. virtual photons).The Casimir force supplies a strong nonlinear perturbation to membrane motion when the membrane-substrate separation is less than 150 nm. Taken together, the unique properties of this system makes it an intriguing candidate for transduction, accelerometry, and sensing applications. / Engineering and Applied Sciences

Nano-structures, such as photonic crystal cavities and metallic antennas, allow one to focus and store optical energy into very small volumes, greatly increasing light-matter interactions. These structures produce resonances which are typically characterized by how well they confine energy both temporally (quality factor–Q) and spatially (mode volume–V). In order to observe non-linear effects, modified spontaneous emission (e.g. Purcell enhancement), or quantum effects (e.g. vacuum Rabi splitting), one needs to maximize the ratio of Q/V while also maximizing the coupling between the resonance and the active medium. In this dissertation I will discuss several projects related by the goal of controlling light-matter interactions using such nano-structures. In the first portion of this dissertation I will discuss the deterministic placement of self-assembled InAs quantum dots, which would allow one to precisely position an optically-active material, for maximum interaction, inside of a photonic crystal cavity. Additionally, I will discuss the use of atomic layer deposition to tune and improve both the resonance wavelength and quality factor of silicon based photonic crystal cavities. Moving from dielectric materials to metals allows one to achieve mode-volumes well below the diffraction limit. The quality factor of these resonators is severely limited by Ohmic loss in the metal; however, the small mode-volume still allows for greatly enhanced light-matter interaction. In the second portion of this dissertation I will investigate the coupling between an array of metallic resonators (antennas) and a nearby semiconductor quantum well. Using time-resolved pump-probe measurements I study the properties of the coupled system and compare the results to a model which allows one to quantitatively compare various antenna geometries.

During the last decade, surface plasmon resonance (SPR) has become widely used to characterize a biological surface and to characterize binding events in the fields of chemistry and biochemistry. Research in this field has been favoured by the tremendous growth in nanofabrication methods among which soft lithographies are alternatively emerging. The purpose of this thesis work was to develop soft UV nanoimprint lithography, an emerging flexible technology allowing patterning on large area of subwavelength photonic nanostructures. The main advantages offered by soft UV nanoimprint lithography concern the simple patterning procedure and the low cost of the experimental setup (see state-of-art presented in chapter 1). Chapters 2 and 3 present the fabrication of master stamps, the study of nanoimprinting parameters coupled with the optimization of the etching process in order to get metallic nanostructures with limited pattern defects. The physical mechanisms of the transmission phenomenon exalted by surface plasmons were studied based on arrays of imprinted gold nanoholes (chapter 4). Extraordinary light transmission has been experimentally demonstrated. The geometrical effects on the position transmission peak were systematically analyzed. Proof-of-concept measurements performed in simple fluidic device indicate a response to small changes in refractive index in the surface vicinity. Finally, chapter 5 proposes a novel design for the optical sensor which is based on "nanocavities" exhibiting coupled localized plasmons. This LSPR sensor offers an improvement of one order of magnitude of the Figure of Merit compared to classical LSPR sensors. The resonance properties of these innovative nanocavities have been studied from numerical simulations and discussed based on their geometrical dependence. Since this system has demonstrated higher sensitivity for detection of biomolecules, it is thus fully adapted to study immunochemical binding interactions.

Photonic cavities are able to confine light to a volume of the order of wavelength of light and this ability can be described in terms of the cavity’s quality factor, which in turn, is proportional to the confinement time in units of optical period. This property of the photonic cavities have been found to be very useful in cavity quantum electrodynamics, for e.g., controlling emission from strongly coupled single photon sources like quantum dots. The smallest possible mode volume attainable by a dielectric cavity, however, poses a limit to the degree of coupling and therefore to the Purcell effect. As metal nanoparticles with plasmonic properties can have mode volumes far below the diffraction limit of light, these can be used to achieve stronger coupling, but the lossy nature of the metals can result in extremely poor quality factors. Hence a hybrid approach, where a high-quality dielectric cavity is combined with a low-quality metal nanoparticle, is being actively pursued. Such structures have been shown to have the potential to preserve the best of both worlds. This thesis describes the design, fabrication and characterization of hybrid plasmonic – photonic nanobeam cavities. Experimentally, we were able to achieve a quality factor of 1200 with the hybrid approach, which suggests that the results are promising for future single photon emission studies. It was found that modeling the behaviour (resonant frequencies, quality factors) of these hybrid cavities with conventional computation methods like FDTD can be tedious, for e.g., a comprehensive study of the electromagnetic fields inside a hybrid photonic nanobeam cavity has been found to take up to 48 hours with FDTD. Hence, we also present an alternate method of analysis using perturbation theory, showing good agreement with FDTD. / Graduate

The linear and nonlinear optical response of plasmon hybridized systems is the subject of study of this thesis. Plasmonic silver nanoprisms are able to confine light to a sub-wavelength volume, which provides local field enhancement. This confined field is promising for achieving an enhanced nonlinear optical response. For many of plasmon nanoparticles, however, the plasmonic resonance is not at the near-infrared wavelengths of a Ti:Sapphire laser, the most common source used for ultra-fast measurements. To achieve resonance at these wavelengths, a tuning mechanism is required. The plasmon hybridization between silver nanoprisms and a thin gold film provides this tuning mechanism, which allows for enhanced optical second harmonic generation. Overlapping the plasmon resonance of the system with excitation source, by varying the spacer layer between the nanoprisms and the gold film, enhances the second harmonic counts by approximately three orders of magnitude. The finite-difference time-domain calculations agree to within a factor of two with the experimental findings in terms of the predicted enhancement factor. This plasmon hybridization approach is promising for future applications, including enhanced multi-photon lithography and nonlinear sensing using metal nanoparticles. / Graduate

The optics and photonics development is currently driven towards nanometer scales. However, diffraction imposes challenges for this development because it prevents confinement of light below a physical limit, commonly known as the diffraction limit. Several implications of the diffraction limit include that conventional optical microscopes are unable to resolve objects smaller than 250nm, and photonic circuits have a physical dimension on the order of the wavelength. Metals at optical frequencies display collective electron oscillations when excited by photon energy, giving rise to the surface plasmon modes with subdiffractional modal profile at metal-dielectric interfaces. Therefore, metallo-dielectric structures are promising candidates for alleviating the obstacles due to diffraction. This thesis investigates a particular branch of plasmonic structures, namely plasmonic antennas, for the purpose of optical imaging and sensing applications. Plasmonic antennas are known for their ability of dramatic near-field enhancement, as well as effective coupling of free-space radiation with localized energy. Such properties are demonstrated in this thesis through two particular applications. The first one is to utilize the interference of evanescent waves from an array of antennas to achieve near-field subdiffraction focusing, also known as superfocusing, in both one and two dimensions. Such designs could alleviate the tradeoffs in the current near-field scanning optical microscopy by improving the signal throughput and extending the imaging distance. The second application is to achieve more efficient radiation from single-emitters through coupling to a highly directive leaky-wave antenna. In this case, the leaky-wave antenna demonstrates the ability of enhancing the directivity over a very wide spectrum.

The optics and photonics development is currently driven towards nanometer scales. However, diffraction imposes challenges for this development because it prevents confinement of light below a physical limit, commonly known as the diffraction limit. Several implications of the diffraction limit include that conventional optical microscopes are unable to resolve objects smaller than 250nm, and photonic circuits have a physical dimension on the order of the wavelength. Metals at optical frequencies display collective electron oscillations when excited by photon energy, giving rise to the surface plasmon modes with subdiffractional modal profile at metal-dielectric interfaces. Therefore, metallo-dielectric structures are promising candidates for alleviating the obstacles due to diffraction. This thesis investigates a particular branch of plasmonic structures, namely plasmonic antennas, for the purpose of optical imaging and sensing applications. Plasmonic antennas are known for their ability of dramatic near-field enhancement, as well as effective coupling of free-space radiation with localized energy. Such properties are demonstrated in this thesis through two particular applications. The first one is to utilize the interference of evanescent waves from an array of antennas to achieve near-field subdiffraction focusing, also known as superfocusing, in both one and two dimensions. Such designs could alleviate the tradeoffs in the current near-field scanning optical microscopy by improving the signal throughput and extending the imaging distance. The second application is to achieve more efficient radiation from single-emitters through coupling to a highly directive leaky-wave antenna. In this case, the leaky-wave antenna demonstrates the ability of enhancing the directivity over a very wide spectrum.