Broad spectral tunability is a desired feature of many photonic and plasmonic components, such as optical filters, semiconductor lasers, and plasmonic materials. Here I show that unique properties of long-range surface plasmon polaritons (LR SPP) allow one to produce optical components with very wide tuning range using small variations in the refractive index of the dielectric cladding material. As a proof-of-concept demonstration, I present operation of LR-SPP-based bandpass optical filters in which a 0.004 variation in the refractive index of the cladding dielectric translates into 210 nm of bandpass tuning at telecom wavelengths. The tuning mechanism proposed here may be used to create monolithic bandpass filters with tuning range spanning over more than an optical octave, compact and widely-tunable diode and quantum cascade laser systems, multi-spectral imagers, and other plasmonic components with broadly-tunable optical response. / text

xiii, 133 p. ; ill. (some col.) A print copy of this title is available through the UO Libraries. Search the library catalog for the location and call number. / We analyze the effect of geometry and surface morphology on the optical properties of metal-dielectric systems. Using both analytical and numerical modeling, we study how surface curvature affects the propagation of surface plasmon polaritons (SPPs) along a metal-dielectric interface. We provide an intuitive explanation for how the curvature causes the phase front to distort, causing the SPPs to radiate their energy away from the metal-dielectric interface. We quantify the propagation efficiency as functions of the radius of curvature, and show that it depends nonmonotonically on the bend radius. We also show how the surface morphology influences the transmittance and the reflectance of light from disordered metal-dielectric nanocomposite films. The films consist of semicontinuous silver films of various surface coverage that are chemically deposited onto glass substrates. They exhibit a large and broadband reflection asymmetry in the visible spectral range. In order to investigate how the surface morphology affects the asymmetry, we anneal the samples at various temperatures to induce changes in the morphology, and observe changes in the reflection spectra. Our study indicates that the surface roughness and the metal surface coverage are the key geometric parameters affecting the reflection spectra, and reveals that the large asymmetry is due to the different surface roughness light encounters when incident from different side of the film. Additionally, we analyze how thin metal and dielectric layers affect the optical properties of metal-dielectric systems. Using the concept of dispersion engineering, we show that a metal-dielectric-metal microsphere--a metal sphere coated with a thin dielectric shell, followed by a metal shell--support a band of surface plasmon resonances (SPRs) with nearly identical frequencies. A large number of modes belonging to this band can be excited simultaneously by a plane wave, and hence enhancing the absorption cross-section. We also find that the enhanced absorption is accompanied by a plasmon assisted transparency due to an avoided crossing of dominant SPR bands. We demonstrate numerically that both the enhanced absorption and the plasmon assisted transparency are tunable over the entire visible range. We also present an experimental study of light scattering from silica spheres coated with thin semicontinuous silver shells, and attempt to describe their optical response using a modified scaling theory. This dissertation includes previously published co-authored materials. / Adviser: Miriam Deutsch

xiii, 129 p. : ill. (some col.) A print copy of this thesis is available through the UO Libraries. Search the library catalog for the location and call number. / Surface plasmon polaritons (SPPs) are collective electron excitations with attendant electromagnetic fields which propagate on a metal-dielectric interface. They behave, in many ways, as model two-dimensional electromagnetic waves. However, because the evanescent field of the SPPs extends a short distance outside the interface, a near-field probe can modify the wave propagation. We use this behavior to study both SPP scattering within the plane of the interface and also the transition to free-space propagation out of the plane. We have, in particular, studied the multiple scattering of SPPs excited on rough silver films. Our laboratory possesses apertureless near-field scanning optical microscopes (A-NSOMs), the probes of which can act as an in-plane scatterer of SPPs. Subsequent momentum-conserving decays of the SPPs generate an expanding hollow cone of light to which information about the direction and phase of the SPPs on the surface is transferred. A focus of our studies has been SPP multiple scattering when one of the scatterers (the tip) can move. This problem is very closely related to a similar problem in mesoscopic electronic transport, involving "universal conductance fluctuations". It is also related to various radar-detection, microwave communications and medical imaging problems. In parallel with actual experimental measurements, we have also conducted extensive Monte Carlo simulations of the scattering. Multiple scattering leads to the appearance and detection of "speckle" in the far field. A speckle field, however, is more properly considered in terms of its embedded optical vortices and so we have used holographic techniques to study these. We have demonstrated that vortices can be manipulated, created and destroyed by movement of the STM probe tip. Optical vortices are an example of the effect of "geometric" or "topological" phase in physics and as such link the trajectory of a parameter in one space to the phase observed in another. In our case, the trajectory of the A-NSOM tip parallel to the sample surface plane generates topological phase in the far field, manifestations of which are vortices. / Committee in charge: Stephen Kevan, Chairperson, Physics; Stephen Gregory, Advisor, Physics; Michael Raymer, Member, Physics; David Strom, Member, Physics; Mark Lonergan, Outside Member, Chemistry

Since Ebbesen's seminal work in 1998 observing extraordinary optical transmission (EOT) through nanohole arrays, much research has focused on the role of surface plasmon polaritons (SPPs) in EOT. While the energy and momentum conditions have become clear, no consensus has been reached on the role of incident light polarization. This study presents a simple model that captures Bloch-SPP excitation, including the role of polarization, in general periodic plasmonic structures. Our model predicts that under certain conditions polarization conversion should occur in EOT light transmitted through the nanohole array. We experimentally measure polarization conversion in EOT and compare the experimentally obtained results to the predictions of our model. Using numerical simulations, we tie the far field experimental results to the near field underlying physics described by our model. In using polarization conversion to provide evidence supporting our model, we also establish a novel approach to achieving polarization conversion based on SPPs instead of hole shape or other techniques in literature, and present reasons why this approach to achieving polarization conversion may be better suited for applications in biomedical sensing and optical elements. / Master of Science / In 1998, Ebbesen et al¹ observed that when light is shown on a metal nanofilm perforated with nanoholes more light appears on the other side of the metal film than was incident on the nanoholes. The unexpectedly high transmission of light through the nanohole array was termed extraordinary optical transmission (EOT), and quickly found applications in diverse fields such as biomedical sensing^13,14, energy harvesting^12,31, and nonlinear optics^12–14,24 . As the importance of EOT in applications became clear, interest developed in understanding the fundamental physics involved. Over the next 20 years, researchers showed that the incident light (made up of electromagnetic fields) excites conduction electrons on the surface of the metal film¹¹ . Specifically, the light and the electrons couple to form quasiparticles known as surface plasmon polaritons (SPP) which propagate along the surfaces of the metal film. The SPPs on the back surface of the metal film then radiate free space transmitted light, which is observed as EOT. However, much of the physics involved how SPPs mediate EOT has remained unclear. The first focus of this work is theoretical, presenting a microscopic model for SPP mediated EOT. In contrast to many groups which aim to characterize SPPs from their far field properties, our model focuses on the near field microscopic physics and presents the far field properties as a consequence of the near field physics. Since the near field cannot be probed iv experimentally, we use numerical simulations to both verify our model’s predictions in the near field and predict the properties that should be measured in the far field. The second focus of this work is more applications driven. We notice that our model predicts that under certain conditions SPPs should cause a phenomenon known as polarization conversion to occur, which is when the polarization of the transmitted light is different from the polarization of the incident light. We experimentally measure the predicted polarization conversion, thereby providing substantial experimental evidence in support of our theoretical model. Our novel approach to achieving polarization conversion based on the behavior of SPPs differs substantially from the approaches in literature (usually based on hole shape²⁴). We present the reasons why our SPP-based approach to achieving polarization conversion is more robust to fabrication imperfections than the conventional approaches, and describe how our approach could affect various applications.

Wavelength-tunable optical response from solid-state optoelectronic devices is a desired feature for a variety of applications such as spectroscopy, laser emission tuning, and telecommunications. Nonlinear optical response, on the other hand, has an important role in modern photonic functionalities, including efficient frequency conversions, all-optical signal processing, and ultrafast switching. This study presents the development of optical devices with wavelength tunable or nonlinear optical functionality based on plasmonic effects. For the first part of this study, widely wavelength tunable optical bandpass filters based on the unique properties of long-range surface plasmon polaritons (LR SPP) are presented. Planar metal stripe waveguides surrounded by two different cladding layers that have dissimilar refractive index dispersions were used to develop a wide wavelength tuning. The concept was demonstrated using a set of index-matching fluids and over 200nm of wavelength tuning was achieved with only 0.004 of index variation. For practical application of the proposed concept, a thermo-optic polymer was used to develop a widely tunable thermo-optic bandpass filter and over 220 nm of wavelength tuning was achieved with only 8 ºC of temperature variation. Another novel approach to produce a widely wavelength tunable optical response for free-space optical applications involves integrating plasmonic metasurfaces with quantum-electronic engineered semiconductor layers for giant electro-optic effect, which is proposed and experimentally demonstrated in the second part of this study. Coupling of surface plasmon modes formed by plasmonic nanoresonators with Stark tunable intersubband transitions in multi-quantum well structures induced by applying bias voltages through the semiconductor layer was used to develop tunable spectral responses in the mid-infrared range. Experimentally, over 310 nm of spectral peak tuning around 7 μm of wavelength with 10 ns response time was achieved. As the final part of this study, highly nonlinear metasurfaces based on coupling of electromagnetically engineered plasmonic nanoresonators with quantum-engineered intersubband nonlinearities are proposed and experimentally demonstrated. In the proof-of-concept demonstration, an effective nonlinear susceptibility over 50 nm/V was measured and, after further optimization, over 480 nm/V was measured for second harmonic generation under normal incidence. The proposed concept shows that it is possible to engineer virtually any element of the nonlinear susceptibility tensor of the nonlinear metasurface. / text

Thesis advisor: Michael J. Naughton / Surface plasmon polaritons (SPPs) are hybridized quasiparticles of photons and electron density waves. They are confined to propagate along metal-dielectric interfaces, and decay exponentially along the direction perpendicular to the interfaces. In the past two decades, SPPs have drawn intensive attention and undergone rapid development due to their potential for application in a vast range of fields, including but not limited to subwavelength imaging, biochemical/biomedical sensing, enhanced light trapping for solar cells, and plasmonic logic gates. These applications utilize the following intrinsic properties of SPPs: (1) the wavelength of SPPs is shorter (and can be much shorter) than that of free photons with the same frequency; (2) the local electric field intensity associated with SPPs can be orders of magnitude larger than that of free photons; and (3) SPPs are bound to metal surfaces, and are thus easily modulated by the geometry of those surfaces. Here, we present studies on SPPs along metal surfaces with novel structures, including the following: (1) SPP standing waves formed along circular metal surfaces that lead to a "plasmonic halo" effect; (2) directional reflectionless conversion between free photons and SPPs in asymmetric metal-insulator-metal arrays; and (3) broadband absorbance enhancement of embedded metallic nanopatterns in a photovoltaic absorber layer. These works may prove useful for new schemes for SPP generation, plasmon-photon modulation, ultrasensitive dielectric/bio sensing, and high efficiency thin film solar cells. / Thesis (PhD) — Boston College, 2014. / Submitted to: Boston College. Graduate School of Arts and Sciences. / Discipline: Physics.

No description available.

Surface plasmon-polaritons are optical surface waves formed through the interaction of photons with free electrons at the surface of metals. They offer interesting applications in a broad range of scientific fields such as physics, chemistry, biology, and material science. However, many of such applications face limitations imposed by the high propagation losses of these waves at visible and near-infrared wavelengths, which result mainly from power dissipation in the metal. In principle, the propagation losses of surface plasmon-polaritons can be compensated through optical amplification. The objective of this thesis is to provide deeper insights on the physics of surface plasmon-polariton amplification and spontaneous emission in surface plasmon-polariton amplifiers through theoretical and experimental vehicles applied (but not necessarily restricted) to a particular plasmonic mode termed long-range surface plasmon-polariton. On the theoretical side, the objective is approached by developing a realistic theoretical model to describe the small-signal amplification of surface plasmon-polaritons in planar structures incorporating dipolar gain media such as organic dye molecules, rare-earth ions, and quantum dots. This model takes into account the inhomogeneous gain distribution formed near the metal surface due to a non-uniform excitation of dipoles and due to a position-dependent excited-state dipole lifetime that results from near-field interactions between the excited dipoles and the metal. Also, a theoretical model to describe the amplified spontaneous emission of surface plasmon-polaritons supported by planar metallic structures is developed. This model takes into account the different energy decay channels into which an exited dipole located in the vicinity of the metal can relax. The validity of this model is confirmed through experimentation. On the experimental side, the objective is approached by providing a direct experimental demonstration of complete loss compensation in a plasmonic waveguide. The experiments are conducted using the long-range surface plasmon-polariton supported by a symmetric thin gold waveguide incorporating optically pumped organic dye molecules in solution as the gain medium. Also, an experimental study of spontaneous emission in a long-range surface plasmon-polariton amplifier is presented. It is shown that this amplifier benefits from a low spontaneous emission into the amplified mode, which leads to an optical amplifier with low noise characteristics. The experimental setup and techniques are explained in detail.

Semiconductor quantum dots and metal nanoparticles feature very strong light-matter interactions, which has led to their use in many photonic applications such as photodetectors, biosensors, components for telecommunications etc.Under illumination both structures exhibit collective electron-photon resonances, described in the frameworks of quasiparticles as exciton-polaritons for semiconductors and surface plasmon-polaritons for metals.To date these two approaches to controlling light interactions have usually been treated separately, with just a few simple attempts to consider exciton-plasmon interactions in a system consisting of both semiconductor and metal nanostructures.In this work, the exciton-polaritons and surface \\plasmon-polaritons are first considered separately, and then combined using the Finite Difference Time Domain numerical method coupled with a master equation for the exciton-polariton population dynamics.To better understand the properties of excitons and plasmons, each quasiparticle is used to investigate two open questions - the source of the Stokes shift between the absorption and luminescence peaks in quantum dots, and the source of the photocurrent increase in quantum dot infrared photodetectors coated by a thin metal film with holes. The combined numerical method is then used to study a system consisting of multiple metal nanoparticles close to a quantum dot, a system which has been predicted to exhibit quantum dot-induced transparency, but is demonstrated to just have a weak dip in the absorption. / <p>QC 20120417</p>

Surface plasmon-polaritons are optical surface waves formed through the interaction of photons with free electrons at the surface of metals. They offer interesting applications in a broad range of scientific fields such as physics, chemistry, biology, and material science. However, many of such applications face limitations imposed by the high propagation losses of these waves at visible and near-infrared wavelengths, which result mainly from power dissipation in the metal. In principle, the propagation losses of surface plasmon-polaritons can be compensated through optical amplification. The objective of this thesis is to provide deeper insights on the physics of surface plasmon-polariton amplification and spontaneous emission in surface plasmon-polariton amplifiers through theoretical and experimental vehicles applied (but not necessarily restricted) to a particular plasmonic mode termed long-range surface plasmon-polariton. On the theoretical side, the objective is approached by developing a realistic theoretical model to describe the small-signal amplification of surface plasmon-polaritons in planar structures incorporating dipolar gain media such as organic dye molecules, rare-earth ions, and quantum dots. This model takes into account the inhomogeneous gain distribution formed near the metal surface due to a non-uniform excitation of dipoles and due to a position-dependent excited-state dipole lifetime that results from near-field interactions between the excited dipoles and the metal. Also, a theoretical model to describe the amplified spontaneous emission of surface plasmon-polaritons supported by planar metallic structures is developed. This model takes into account the different energy decay channels into which an exited dipole located in the vicinity of the metal can relax. The validity of this model is confirmed through experimentation. On the experimental side, the objective is approached by providing a direct experimental demonstration of complete loss compensation in a plasmonic waveguide. The experiments are conducted using the long-range surface plasmon-polariton supported by a symmetric thin gold waveguide incorporating optically pumped organic dye molecules in solution as the gain medium. Also, an experimental study of spontaneous emission in a long-range surface plasmon-polariton amplifier is presented. It is shown that this amplifier benefits from a low spontaneous emission into the amplified mode, which leads to an optical amplifier with low noise characteristics. The experimental setup and techniques are explained in detail.