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This thesis presents a Hamiltonian formulation of the electromagnetic fields in structured (inhomogeneous) media of arbitrary dimensionality, with arbitrary material dispersion and absorption consistent with causality. The method is based on an identification of the photonic component of the polariton modes of the system. Although the medium degrees of freedom are introduced in an oscillator model, only the macroscopic response of the medium appears in the derived eigenvalue equation for the polaritons. For both the discrete transparent-regime spectrum and the continuous absorptive-regime spectrum, standard codes for photonic modes in nonabsorptive systems can easily be leveraged to calculate polariton modes. Two applications of the theory are presented: pulse propagation and spontaneous parametric down-conversion (SPDC). In the propagation study, the dynamics of the nonfluctuating part of a classical-like pulse are expressed in terms of a Schr\"{o}dinger equation for a polariton effective field. The complex propagation parameters of that equation can be obtained from the same generalized dispersion surfaces typically used while neglecting absorption, without incurring additional computational complexity. As an example I characterize optical pulse propagation in an Au/MgF$_2$ metallodielectric stack, using the empirical response function, and elucidate the various roles of Bragg scattering, interband absorption and field expulsion. Further, I derive the Beer coefficient in causal structured media. The SPDC calculation is rigorous, captures the full 3D physics, and properly incorporates linear dispersion. I obtain an expression for the down-converted state, quantify pair-production properties, and characterize the scaling behavior of the SPDC energy. Dispersion affects the normalization of the polariton modes, and calculations of the down-conversion efficiency that neglect this can be off by 100$\%$ or more for common media regardless of geometry if the pump is near the band edge. Furthermore, I derive a 3D three-wave group velocity walkoff factor; due to the interplay of a topological property with a symmetry property, I show that even if down-conversion is into a narrow forward cone, neglect of the transverse walkoff can lead to an overestimate of the SPDC energy by orders of magnitude.

This thesis presents a Hamiltonian formulation of the electromagnetic fields in structured (inhomogeneous) media of arbitrary dimensionality, with arbitrary material dispersion and absorption consistent with causality. The method is based on an identification of the photonic component of the polariton modes of the system. Although the medium degrees of freedom are introduced in an oscillator model, only the macroscopic response of the medium appears in the derived eigenvalue equation for the polaritons. For both the discrete transparent-regime spectrum and the continuous absorptive-regime spectrum, standard codes for photonic modes in nonabsorptive systems can easily be leveraged to calculate polariton modes. Two applications of the theory are presented: pulse propagation and spontaneous parametric down-conversion (SPDC). In the propagation study, the dynamics of the nonfluctuating part of a classical-like pulse are expressed in terms of a Schr\"{o}dinger equation for a polariton effective field. The complex propagation parameters of that equation can be obtained from the same generalized dispersion surfaces typically used while neglecting absorption, without incurring additional computational complexity. As an example I characterize optical pulse propagation in an Au/MgF$_2$ metallodielectric stack, using the empirical response function, and elucidate the various roles of Bragg scattering, interband absorption and field expulsion. Further, I derive the Beer coefficient in causal structured media. The SPDC calculation is rigorous, captures the full 3D physics, and properly incorporates linear dispersion. I obtain an expression for the down-converted state, quantify pair-production properties, and characterize the scaling behavior of the SPDC energy. Dispersion affects the normalization of the polariton modes, and calculations of the down-conversion efficiency that neglect this can be off by 100$\%$ or more for common media regardless of geometry if the pump is near the band edge. Furthermore, I derive a 3D three-wave group velocity walkoff factor; due to the interplay of a topological property with a symmetry property, I show that even if down-conversion is into a narrow forward cone, neglect of the transverse walkoff can lead to an overestimate of the SPDC energy by orders of magnitude.

xx, 162 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. / In this thesis we theoretically and experimentally investigate the subwavelength manipulation of light with nano-scale patterned metallodielectric resonators. By coupling light to surface plasmon excitations, we calculate the modified dispersion relation of the resulting surface plasmon polariton (SPP) modes in two types of subwavelength resonators: (i) closed, spherical micro-resonators with nano-scale metal-dielectic-metal shells; (ii) periodic, metal-dielectric-metal-layered silica surfaces. We show theoretically that with the proper geometric parameters, one can use sub-wavelength structure on spherical surfaces to manipulate the SPP dispersion relation in a highly tunable fashion. A tunable avoided-crossing of plasmonic dispersion bands is found to be the result of the coherent near-field coupling of silver nano-shell SPP modes. By developing our own stable computational algorithms, we calculated the far-field scattering of these metal-dielectric-metal layered micro-resonators. We demonstrate that the near-field interaction of the SPPs leads to a tunable, SPP induced transparency in the composite particle's scattering and extinction cross-sections. Utilizing finite element calculations, periodically-modulated metal-dielectric-metal layers are shown to alter the transmission properties of plasmon enhanced transmission through their support of interior surface plasmon (ISP) modes. Our simulations indicate that, subwavelength silver-silica-silver trilayers coating arrays of silica cylinders support ISP modes analogous to those found in spherical metal-dielectric-metal shells. We examine the coupling between ISP and radiating SPPs, and find the possibility of efficient free-space coupling to ISP modes in planar geometries. Further, the excitation of these ISP modes is found to predicate plasmon enhanced transmission, adding directionality and refined frequency selection. Experimentally, we show that self-assembled monolayers of silica spheres form a novel substrate for tunable plasmonic surfaces. We have developed a deposition method to conformally coat these hexagonal-close-packed substrates with nano-scale silver-polystyrene-silver coatings. We use angle-resolved spectroscopy to study their transmission properties. We have discovered that the presence of the silver-polystyrene-silver layer supports the excitation of ISP modes, and that these excitations significantly alter the plasmon enhanced transmission. Finally, we have discovered that the use of the ordered monolayers as a plasmonic substrate can create a new effect in conjunction with plasmon enhanced transmission: directionally asymmetric transmission. This is demonstrated with optically thick silver coatings evaporated upon onto the ordered sphere monolayers. / Adviser: Miriam Deutsch

<p>The resonance of surface plasmons on metal nanoparticles can be excited at visible wavelengths. The extraordinary enhancement of a variety of optical phenomena in the vicinity of metal nanoparticles has been attributed to the strong fields generated under resonance conditions. As a result, extensive research has been carried out to incorporate the extraordinary optical properties of metal nanoparticles into optical devices and applications, ranging from spectroscopy (e.g, surface enhanced Raman, IR and Fluorescence), optical sensing and imaging, to photovoltaic cells, photonic crystals and optical switches. Particular effort has been directed towards producing stable dispersion of metal nanoparticles within soft dielectric matrices and their subsequent construction into different device geometries.</p> <p>This thesis describes a method to photolytically generate Ag nanoparticles within organosiloxane sols, which can subsequently be photopolymerized in the presence of photoinitiators and therefore, be patterned through a variety of photo-inscription processes. The mechanism of Ag nanoparticle growth and evolution is described in detail followed by the fabrication of periodic metallodielectric gratings through photomask and laser interference lithography. Studies also showed that three different forms of nonlinear light propagation, optical self-trapping, modulation instability and spatial self-phase modulation could be elicited in the Ag nanoparticle-doped systems. Detailed experimental examination of these phenomena elucidated significant differences in their dynamics in the metallodielectric systems compared to non-doped samples. These included variations in the dynamics of self-trapped beams such as the excitation of optical modes, critical thresholds for modulation instability and self-phase modulation. The potential of these nonlinear processes for the self-inscription of 3-D metallodielectric structures including cylindrical multimode waveguides and waveguide lattices has also been studied.</p> / Doctor of Philosophy (PhD)

Studies of the radiative properties of thin films and near-field radiation transfer in layered structures are important for applications in energy, near-field imaging, coherent thermal emission, and aerospace thermal management. A comprehensive study is performed on the optical constants of dielectric tantalum pentoxide (Ta₂O₅) and hafnium oxide (HfO₂) thin films from visible to the far infrared using spectroscopic methods. These materials have broad applications in metallo-dielectric multilayers, anti-reflection coatings, and coherent emitters based on photonic crystal structures, especially at high temperatures since both materials have melting points above 2000 K. The dielectric functions of HfO₂ and Ta₂O₅ obtained from this work may facilitate future design of devices with these materials. A parametric study of near-field TPV performance using a backside reflecting mirror is also performed. Currently proposed near-field TPV devices have been shown to have increased power throughput compared to their far-field counterparts, but whose conversion efficiencies are lower than desired. This is due to their low quantum efficiency caused by recombination of minority carriers and the waste of sub-bandgap radiation. The efficiency may be improved by adding a gold mirror as well as by reducing the surface recombination velocity, as demonstrated in this thesis. The analysis of the near-field TPV and proposed methods may facilitate the development or high-efficiency energy harvesting devices. Many near-field devices may eventually utilize metallo-dielectric structures which exhibit unique properties such as negative refraction due to their hyperbolic isofrequency contour. These metamaterials are also called indefinite materials because of their ability to support propagating waves with large lateral wavevectors, which can result in enhanced near-field radiative heat transfer. The energy streamlines in such structures are studied for the first time. Energy streamlines illustrate the flow of energy through a structure when the fields are evanescent and energy propagation is not ray like. The energy streamlines through two semi-infinite uniaxially anisotropic effective medium structures, separated by a small vacuum gap, are modeled using the Green’s function. The lateral shift and penetration depth are calculated from the streamlines and shown to be relatively large compared to the vacuum gap dimension. The study of energy streamlines in hyperbolic metamaterials helps understand the near-field energy propagation on a fundamental level.