This thesis examines the feasibility of using conventional semiconductors, specifically GaAs, as a plasmonic material at the operating wavelength of 1550nm, due to its many merits such as achievable low losses and mature micro-fabrication technologies. A theoretical study is performed on GaAs that yielded the condition for plasmonic behaviour at a minimum free carrier density of 7.2 x 10^20cm^-3 in bulk materials. The most feasible route to achieving this condition is determined to be intense optical excitation, and the required intensity considering a 150fs pulse at the above bandgap wavelength of 870nm is approximately 2.55TW/cm^2. A Bragg reflection ridge waveguide (BRW) using GaAs-AlGaAs is designed and micro-fabricated, and a counter-propagating pump-probe experiment is devised to test the plasmonic effect using the BRW. Results from two different ultrafast lasers include the observation of pump (870nm and 800nm) coupling to fundamental Bragg modes, and the measurement of the pump transmission spectrum.

This thesis examines the feasibility of using conventional semiconductors, specifically GaAs, as a plasmonic material at the operating wavelength of 1550nm, due to its many merits such as achievable low losses and mature micro-fabrication technologies. A theoretical study is performed on GaAs that yielded the condition for plasmonic behaviour at a minimum free carrier density of 7.2 x 10^20cm^-3 in bulk materials. The most feasible route to achieving this condition is determined to be intense optical excitation, and the required intensity considering a 150fs pulse at the above bandgap wavelength of 870nm is approximately 2.55TW/cm^2. A Bragg reflection ridge waveguide (BRW) using GaAs-AlGaAs is designed and micro-fabricated, and a counter-propagating pump-probe experiment is devised to test the plasmonic effect using the BRW. Results from two different ultrafast lasers include the observation of pump (870nm and 800nm) coupling to fundamental Bragg modes, and the measurement of the pump transmission spectrum.

Nanophotonics, especially plasmonics is a kind of very active research area, which deals with the interaction behavior between electromagnetic radiation and metallic nanostructures. It has attracted enormous attention over recent decades due to its great potential of ripple effects on electronics, energy, environmental, and medical industries as well as scientific interests. In particular, noble metal nanoparticles exhibit localized surface plasmon resonance (LSPR), which is the collective oscillating excitation of the free electrons on the surface of metal nanoparticles when light is incident on the particle. The LSPR extinction peak is very sensitive to the dielectric environment near the particle surface and can be tailored by the particle's sizes and shapes. These properties allow LSPR-active substrate using plasmonic gold nanoparticles to be a great transducer for biosensing with real-time and label-free measurement. In addition, the plasmonic gold nanoparticles such as gold nanorod and bipyramid are prepared by the seed-mediated and surfactant-directed method based on the cetyltrimethylammonium bromide (CTAB), which has a great influence on the synthesis. In the growth mechanism, it is believed that CTAB interacts with different facet and defects on the growing nanoparticles to produce different rate of gold ion reduction onto the nanoparticles to generate anisotropic growth. Therefore, CTAB layer is greatly interesting because the modification of nanoparticles surface chemistry is essential to biological targeting, film formation, and assembly of complex structures. Surface enhanced Raman spectroscopy (SERS) of gold nanorods in CTAB solution has been used to analyze a surfactant structural transition based on the distance dependent electromagnetic enhancement. As the surfactant concentration in the gold nanorod solution was reduced, a structural transition in the surfactant layer between 2 mM and 5 mM CTAB solution was observed through a sudden increase in the signal from the alkane chains. A structural transition in the CTAB layer that stabilizes gold nanorods was identified by comparing the intensities of different bands within the CTAB molecule. Therefore, the surface manipulation and analysis of the nanostructures and their interface with controlled environment provide important insight into their structural function and interpretation, and many opportunities for biomedical applications.

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.

Plasmonic nanoparticles support surface plasmon resonances that are sensitive to the environment. Factors contributing to the refractive index sensitivity are explored systematically through simulation, theory, and experiment. Particles small with respect to the wavelength of light and with size parameters much less than 1 have optical properties accurately predicted by quasi-electrostatic theory while particles with larger size parameters necessitate electrodynamics. A theory is developed that captures the effects of geometry on the refractive index sensitivity with a single factor, plasmon band location, and, although based on electrostatic theory, well predicts the sensitivity of particles whose properties are beyond the electrostatic limit. This theory is validated by high quality simulations for compact particles with shape parameters approaching 1 and, therefore, electrodynamic in nature, as well as higher aspect ratio particles that are electrostatic. Experimentally observed optical spectra for nanorods immobilized on glass and subjected to changes in n of the medium are used to calculate the sensitivity of the particles, found to be well matched by a variation on the homogeneous plasmon band theory. The separate electrostatic and electrodynamic components of plasmon band width, are explored and the overall width is found to affect the observability of the aforementioned sensitivity similarly within each particle class. The extent of the sensing volume around a spherical particle is explored and found to vary with particle size for small particles. Through simulation of oriented dielectric layers, it is shown particles are most sensitive to material located in regions of highest field enhancement. Variations on seed-mediated growth of gold nanorods results in spectra exhibiting a middle peak, intermediate to the generally accepted longitudinal and transverse modes. Simulated optical properties and calculated field enhancement illustrates the correlation between geometry and optical properties and allows for identification of the middle peak. / Dissertation

Nowadays plasmonics is rapidly developing areas from fundamental studies to more application driven research. This dissertation contains three different research topics on plasmonics. In the first research topic, by modulating the zone width of a plasmonic zone plate, we demonstrate that a beam focused by a proposed plasmonic zone plate lens can be achieved with higher intensity and smaller spot size than the diffraction-limited conventional zone plate lens. This sub-diffraction focusing capability is attributed to extraordinary optical transmission, which is explained by the complex propagation constant in the zone regions afforded by higher refractive index dielectric layer and surface plasmons. On the other hand, the resulted diffraction efficiency of this device is relatively low. By introducing a metal/dielectric multilayered zone plate, we present higher field enhancement at the focal point. This higher field enhancement originates not only from surface plasmon polaritons-assisted diffraction process along the propagation direction of the incident light (longitude mode), but also from multiple scattering and coupling of surface plasmons along the metal/dielectric interface (transverse mode). In the second research topic, we suggest a novel concept of SERS-active substrate applications. The surface-enhanced Raman scattering enhancement factor supported by gap surface plasmon polaritons is introduced. Due to higher effective refractive index induced by gap surface plasmon polaritons in the spacer region between two metal plates, incident light tends to localize itself mostly in the medium with higher refractive index than its adjacent ones and thereby the lights can confine with larger field enhancement. In the last research topic, we offer a simple structure in which a gold dipole antenna is formed on the SiC substrate. Surface phonon polaritons, counterparts of surface plasmon polaritons in the mid-infrared frequencies, are developed. Due to the synergistic action between the conventional dipole antenna coupling and the resonant excitation of surface phonon polaritons, strong field enhancement in the gap region of dipole antenna is attained. Most of research topics above are expected to find promising applications such as maskless nanolithography, high resolution scanning optical microscopy, optical data storage, optical antenna, SERS-active substrate, bio-molecular sensing and highly sensitive photo-detectors.

Metallic nanostructures that employ localized surface plasmon resonances to capture or radiate electromagnetic waves at optical frequencies are termed "plasmonic optical antennas". These structures enhance light-matter interactions in an efficient manner, enabling unique linear and nonlinear optical applications. One such application is surface-enhanced Raman scattering (SERS), which employs plasmonic antennas to enhance Raman cross-section of molecules by orders of magnitude. SERS has attracted a significant amount of research attention since it enables molecules to be identified through their characteristic vibrational spectra, even at the single molecule level. / Engineering and Applied Sciences

Plasmonic waves in solid-state are caused by collective oscillation of mobile charges inside or at the surface of conductors. In particular, surface plasmonic waves propagating at the skin of metals have recently attracted interest, as they reduce the wavelength of electromagnetic waves coupled to them by up to ~10 times, allowing one to create miniaturized wave devices at optical frequencies. In contrast, plasmonic waves on two-dimensional (2D) conductors appear at much lower infrared and THz-GHz frequencies, near or in the electronics regime, and can achieve far stronger wavelength reduction factor reaching well above 100. In this thesis, we study the unique machinery of 2D plasmonic waves behind this ultra-subwavelength confinement and explore how it can be used to create various interesting devices. To this end, we first develop a physically intuitive theoretical formulation of 2D plasmonic waves, whose two main components---the Coulomb restoration force and inertia of the collectively oscillating charges---are combined into a transmission-line-like model. We then use this formulation to create various ultra-subwavelength 2D plasmonic devices. For the 2D conductor, we first choose GaAs/AlGaAs heterostructure---a 2D electron gas consisting of massive (m*>0) electrons---demonstrating plasmonic bandgap crystals, interferometers, and negatively refracting metamaterials. We then examine a 2D plasmonic device based on graphene, a 2D electron gas consisting of effectively massless (m*=0) electrons. We theoretically show and experimentally demonstrate that the massless electrons in graphene can surprisingly exhibit a collective mass when subjected to a collective excitation, providing the inertia that is essential for the propagation of 2D plasmonic waves. Lastly, we theoretically investigate the thermal current fluctuation behaviors in massive and massless electron gases. While seemingly unrelated on first sight, we show that the thermal current fluctuation is actually intimately linked to the collective mass of the massive or massless electron gas. Thus, we show that the thermal current fluctuation behaviors can also be described by the same theoretical framework introduced earlier, suggesting a possibility to design new concept devices and experiments based on this linkage. / Engineering and Applied Sciences

Two experiments explore the application of plasmonic nanoparticles to cellular pathology. The first devised a platform by which gold-silver nanoparticles act as differentiable labels for cell surface receptors under dark field imaging. By conjugating particles of various constitutions with receptor-targeting antibodies, particles scatter characteristically according to their plasmon peak. The second experiment programmed receptor placement via the patterning of two substrates and used the binding of SERS nanoparticles to explore the quantification of such targets at high-density. On one substrate, anchor pairs established receptors at specified distances in order to define the relationship between scattering intensity and the distance between SERS particles. On the second, anchor regions are filled with increasing densities of receptors and the particle-saturated substrates are probed to relate scattering intensity to particle density. This should discover the density-threshold between linear and non-linear scattering and inform the quantification of particles in the exponential density regime.

Two experiments explore the application of plasmonic nanoparticles to cellular pathology. The first devised a platform by which gold-silver nanoparticles act as differentiable labels for cell surface receptors under dark field imaging. By conjugating particles of various constitutions with receptor-targeting antibodies, particles scatter characteristically according to their plasmon peak. The second experiment programmed receptor placement via the patterning of two substrates and used the binding of SERS nanoparticles to explore the quantification of such targets at high-density. On one substrate, anchor pairs established receptors at specified distances in order to define the relationship between scattering intensity and the distance between SERS particles. On the second, anchor regions are filled with increasing densities of receptors and the particle-saturated substrates are probed to relate scattering intensity to particle density. This should discover the density-threshold between linear and non-linear scattering and inform the quantification of particles in the exponential density regime.