Plasmonic structures with nanometer scale gaps provide localized field enhancement and allow for engineering of the optical response, which is well described by conventional classical models. For subnanometer scale gaps, quantum effects and nonlocal effects become important and classical electromagnetics fail to describe the plasmonic coupling response. Coupled plasmonic system of gold nanoparticles on top of thin gold film separated with self-assembled monolayers (SAMs) provides a convenient geometry to experimentally explore plasmonic features in subnanometer scale gaps. However, the surface roughness of the thin metal film can significantly influence the plasmonic coupling properties. In this dissertation, I suggest modifying the coupled nanoparticles-film structures by using ultraflat thin metal films. Using these structures, I investigated the far-field optical response for gap size variations by dark field scattering measurements. A red-shift of the plasmon resonance wavelength was observed by reducing the gap width. However, I did not observe the previously reported saturation trend of the resonance shift for subnanometer scale gaps. I attribute the difference to surface roughness effects in past works since as they were not present in my studies with ultraflat films. To study the near-field enhancement in subnanometer scale gaps, I used third harmonic generation as a method that is highly sensitive (as the third power) to the local field intensity. The onset of the quantum tunneling regime was determined for gap thicknesses of 0.51 nm, where there was a sudden drop in the third harmonic when the gap width decreases from 0.69 nm to 0.51 nm. The experimental observations were consistent with analytical calculations that applied the quantum-corrected model for SAM separating two gold regions. In comparison to the gap without SAMs in which the onset of the tunneling regime was reported at 0.31 nm, the onset of tunneling across the gap with SAM occurred for larger gaps. This was an expected outcome because the material in the gap reduced the barrier height to tunneling. Furthermore, I investigated the wavelength dependence of the third harmonic generation for the gold plasmonic system to determine the role of the interband transitions in the nonlinear response of gold. Past works reported a strong wavelength dependence of the nonlinear response of gold for the fundamental wavelength at about 550 nm, attributed to the interband transitions between the 5d to 6s-6p bands. However, the roles of the interband transitions and wavelength-dependent field enhancement in the nonlinear response of gold was not investigated. In this dissertation, results showed the third harmonic generation enhanced by an order of magnitude by the interband transition (as compared to the non-resonant case). In my research I also used an analytic model for the dielectric function of gold in which contributions of the interband transitions were considered. This model was also consistent with the experimental observations. / Graduate / 0752 / 0544 / Ghazal.hajisalem@gmail.com

Plasmonic structures are utilized in many applications ranging from bio-medicine to solar energy generation and transfer. Numerical schemes capable of solving equations of classical electrodynamics have been the method of choice for characterizing scattering properties of such structures. However, as dimensions of these plasmonic structures reduce to nanometer scale, quantum mechanical effects start to appear. These effects cannot be accurately modeled by available classical numerical methods. One of these quantum effects is the tunneling, which is observed when two structures are located within a sub-nanometer distance of each other. At these small distances electrons “jump" from one structure to another and introduce a path for electric current to flow. Classical equations of electrodynamics and the schemes used for solving them do not account for this additional current path. This limitation can be lifted by introducing an auxiliary tunnel with material properties obtained using quantum models and applying a classical solver to the structures connected by this auxiliary tunnel. Early work on this topic focused on quantum models that are generated using a simple one-dimensional wave function to find the tunneling probability and assume a simple Drude model for the permittivity of the tunnel. These tunnel models are then used together with a classical frequency domain solver. In this thesis, a time domain surface integral equation solver for quantum corrected analysis of transient plasmonic interactions is proposed. This solver has several advantages: (i) As opposed to frequency domain solvers, it provides results at a broad band of frequencies with a single simulation. (ii) As opposed to differential equation solvers, it only discretizes surfaces (reducing number of unknowns), enforces the radiation condition implicitly (increasing the accuracy), and allows for time step selection independent of spatial discretization (increasing efficiency). The quantum model of the tunnel is obtained using density functional theory (DFT) computations, which account for the atomic structure of materials. Accuracy and applicability of this (quantum corrected) time domain surface integral equation solver will be shown by numerical examples.

Choline oxidase catalyzes the oxidation of choline to glycine betaine. The reaction includes betaine aldehyde as an intermediate. FAD is reduced by the alcohol substrate, betaine aldehyde intermediate and oxidized by molecular oxygen to give hydrogen peroxide. In this study, the Ser101Ala variant of choline oxidase was prepared to elucidate the contribution of the hydroxyl group of Ser101 in the proton and hydride transfer reactions for proper preorganization and reorganization of the active site towards quantum mechanical tunneling. The thermodynamic parameters associated with the enzyme-catalyzed OH and CH bond cleavages and the temperature dependence of the associated solvent and substrate kinetic isotope effects were investigated using a stopped-flow spectrophotometer. The proton and hydride transfer have been shown to be occurring via quantum tunneling in CHO-S101A enzyme.

In this dissertation, I have studied four theoretical problems in quantum tunneling, quantum computing, and high-temperature superconductivity. I have developed a generally-useful numerical tool for analyzing impurity-induced resonant-state images observed with scanning tunneling microscope (STM) in high temperature superconductors. The integrated tunneling intensities on all predominant sites have been estimated. The results can be used to test the predictions of any tight-binding model calculation. I have numerically simulated two-dimensional time-dependent tunneling of a Gaussian wave packet through a barrier, which contains charged ions. We have found that a negative ion in the barrier directly below the tunneling tip can deflect the tunneling electrons and drastically reduce the probability for them to reach the point in the target plane directly below the tunneling tip. I have studied an infinite family of sure-success quantum algorithms, which are introduced by C.-R. Hu [Phys. Rev. A {\bf 66}, 042301 (2002)], for solving a generalized Grover search problem. Rigorous proofs are found for several conjectures made by Hu and explicit equations are obtained for finding the values of two phase parameters which make the algorithms sure success. Using self-consistent Hartree-Fock theory, I have studied an extended Hubbard model which includes quasi-long-range Coulomb interaction between the holes (characterized by parameter V). I have found that for sufficiently large V/t, doubly-charged-antiphase-island do become energetically favored localized objects in this system for moderate values of U/t, thus supporting a recent conjecture by C.-R. Hu [Int. J. Mod. Phys. B {\bf 17}, 3284 (2003)].

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No description available.

This work describes a model of the piezoresistive behavior in nanocomposite sensors. These sensors are also called flexible sensors because the polymer matrix allows for large deformations without failure. The sensors have conductive nanoparticles dispersed through an insulative polymer matrix. The insulative polymer gaps between nanoparticles are assumed to be possible locations for electron tunneling. When the distance between two nanoparticles is small enough, electrons can tunnel from one nanoparticle to the next and ultimately through the entire sensor. The evolution of this gap distance with strain is important to understand the overall conductivity of the strain sensor. The gap evolution was modeled in two ways: (1) applying Poisson's contraction to the sensor as a homogenous material, referred to as Simple Poisson's Contraction (SPC) and (2) modeling the nanoparticle-polymer system with Finite Element Analysis (FEA). These two gap evolution models were tested in a random resistor network model where each polymer gap was treated as a single resistor in the network. The overall resistance was calculated by solving the resistor network system. The SPC approach, although much simpler, was sufficient for cases where various orientations of nanoparticles were used in the same sensor. The SPC model differed significantly from the FEA, however, in cases where nanoparticles had specific alignment, e.g. all nanoparticles parallel to the tensile axis. It was also found that the distribution used to determine initial gap sizes for the polymer gaps as well as the mean of that distribution significantly impacted the overall resistivity of the sensor.Another key part of this work was to determine if the piezoresistivity in the sensors follows a percolation type behavior under strain. The conductance versus strain curve showed the characteristic s-curve behavior of a percolative system. The conductance-strain curve was also compared to the effective medium and generalized effective medium equations and the latter (which includes percolation theory) fit the random resistor network much more closely. Percolation theory is, therefore, an accurate way to describe this polymer-nanoparticle piezoresistive system.Finally, the FEA and SPC models were compared against experimental data to verify their accuracy. There are also two design problems addressed: one to find the sensor with the largest gauge factor and another to determine how to remove the characteristic initial spike in resistivity seen in nanocomposite sensors.

Nesta dissertação são explorados efeitos clássicos e semi-clássicos em espaços-tempos quase-extremos. Na classe de geometrias tratadas aqui, uma região estática entre dois horizontes é considerada, de forma que estes horizontes estão muito próximos e as suas gravidades superficiais são muito pequenas. Este limite quase-extremo surge em vários contextos de interesse, envolvendo buracos negros assintoticamente de Sitter, buracos de minhoca e buracos negros em universos com seção espacial compacta. No trabalho desenvolvido, buracos de minhoca ligando duas regiões com horizontes cosmológicos são estudados em detalhes. Uma vez caracterizada, algumas das propriedades clássicas destas estruturas e efeitos semi-clássicos são explorados. O tratamento quântico proposto leva naturalmente a uma caracterização termodinâmica associada aos horizontes atrapantes presentes na geometria. Consideramos especificamente propriedades térmicas associadas a um campo escalar nos espaços-tempos de interesse. Uma revisão do formalismo de Hayward é feito, com a sua adaptação para espaços-tempos importantes. Buracos de minhoca no regime quase-extremo são discutidos em detalhes. / In this dissertation, classical and semi-classical effects in quasi-extreme spacetimes are explored. In the class of geometries treated here, a static region between two horizons is considered, in such a way that these horizons are very close and their surface gravities are very small. This quasi-extreme limit appears in several contexts of interest, such as asymptotically de Sitter black holes, wormholes and black holes in universes with compact spatial section. In the developed work, wormholes connecting two regions bounded by cosmological horizons are studied in detail. Once some of the classical properties of these structures are characterized, semi-classical effects are explored. The proposed quantum treatment naturally leads to a thermodynamic characterization associated to the trapping horizons present in the geometry. We specifically consider thermal properties associated to a scalar field in the spacetimes of interest. A review of Hayward\'s formalism is presented, with a proper adaptation to important space-times. Wormholes in the near extreme regime are discussed in detail.

abstract: What can classical chaos do to quantum systems is a fundamental issue highly relevant to a number of branches in physics. The field of quantum chaos has been active for three decades, where the focus was on non-relativistic quantumsystems described by the Schr¨odinger equation. By developing an efficient method to solve the Dirac equation in the setting where relativistic particles can tunnel between two symmetric cavities through a potential barrier, chaotic cavities are found to suppress the spread in the tunneling rate. Tunneling rate for any given energy assumes a wide range that increases with the energy for integrable classical dynamics. However, for chaotic underlying dynamics, the spread is greatly reduced. A remarkable feature, which is a consequence of Klein tunneling, arise only in relativistc quantum systems that substantial tunneling exists even for particle energy approaching zero. Similar results are found in graphene tunneling devices, implying high relevance of relativistic quantum chaos to the development of such devices. Wave propagation through random media occurs in many physical systems, where interesting phenomena such as branched, fracal-like wave patterns can arise. The generic origin of these wave structures is currently a matter of active debate. It is of fundamental interest to develop a minimal, paradigmaticmodel that can generate robust branched wave structures. In so doing, a general observation in all situations where branched structures emerge is non-Gaussian statistics of wave intensity with an algebraic tail in the probability density function. Thus, a universal algebraic wave-intensity distribution becomes the criterion for the validity of any minimal model of branched wave patterns. Coexistence of competing species in spatially extended ecosystems is key to biodiversity in nature. Understanding the dynamical mechanisms of coexistence is a fundamental problem of continuous interest not only in evolutionary biology but also in nonlinear science. A continuous model is proposed for cyclically competing species and the effect of the interplay between the interaction range and mobility on coexistence is investigated. A transition from coexistence to extinction is uncovered with a non-monotonic behavior in the coexistence probability and switches between spiral and plane-wave patterns arise. Strong mobility can either promote or hamper coexistence, while absent in lattice-based models, can be explained in terms of nonlinear partial differential equations. / Dissertation/Thesis / Ph.D. Electrical Engineering 2012

Nesta dissertação são explorados efeitos clássicos e semi-clássicos em espaços-tempos quase-extremos. Na classe de geometrias tratadas aqui, uma região estática entre dois horizontes é considerada, de forma que estes horizontes estão muito próximos e as suas gravidades superficiais são muito pequenas. Este limite quase-extremo surge em vários contextos de interesse, envolvendo buracos negros assintoticamente de Sitter, buracos de minhoca e buracos negros em universos com seção espacial compacta. No trabalho desenvolvido, buracos de minhoca ligando duas regiões com horizontes cosmológicos são estudados em detalhes. Uma vez caracterizada, algumas das propriedades clássicas destas estruturas e efeitos semi-clássicos são explorados. O tratamento quântico proposto leva naturalmente a uma caracterização termodinâmica associada aos horizontes atrapantes presentes na geometria. Consideramos especificamente propriedades térmicas associadas a um campo escalar nos espaços-tempos de interesse. Uma revisão do formalismo de Hayward é feito, com a sua adaptação para espaços-tempos importantes. Buracos de minhoca no regime quase-extremo são discutidos em detalhes. / In this dissertation, classical and semi-classical effects in quasi-extreme spacetimes are explored. In the class of geometries treated here, a static region between two horizons is considered, in such a way that these horizons are very close and their surface gravities are very small. This quasi-extreme limit appears in several contexts of interest, such as asymptotically de Sitter black holes, wormholes and black holes in universes with compact spatial section. In the developed work, wormholes connecting two regions bounded by cosmological horizons are studied in detail. Once some of the classical properties of these structures are characterized, semi-classical effects are explored. The proposed quantum treatment naturally leads to a thermodynamic characterization associated to the trapping horizons present in the geometry. We specifically consider thermal properties associated to a scalar field in the spacetimes of interest. A review of Hayward\'s formalism is presented, with a proper adaptation to important space-times. Wormholes in the near extreme regime are discussed in detail.