The absorption of the energy in the form of heat from electromagnetic radiation is strongly dependent on the shape of the surface. Also, the transfer of this generated thermal energy is dependent on the surface area of the object in contact with the surrounding medium. Here in this thesis, we present a structural optimization method for metal nanostructures based on the shape dependency of their electromagnetic heat dissipation and thermodynamic transfer to the surroundings. We have used a parallel genetic algorithm (GA) in conjunction with a coupled electromagnetic (FDTD) and thermodynamic modeling of the metallic nanostructures for the optimization. The optimized nano-structure demonstrates significant improvement in electromagnetic heating in the spectral window of optimization as well as expedited cooling properties. The symmetry of the structures which is inherent in the design procedure makes them independent of the polarization at normal incidence and insensitive to the azimuthal direction of incidence.

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Transparent conducting oxides (TCOs) usually have high conductivity and transparency in the visible range and have been widely used in daily life. Recently, TCOs have attracted great interest due to their potential applications in various new optical and electrical devices (flat-panel displays, energy efficient windows, etc.). Nanostructured TCOs can induce new size related properties, for example, when sizes of TCOs are controlled at the nanometer scale, various defects can introduce different defect-related optical emissions. These new nanostructured TCOs combining traditional and new size dependent properties may be used for construction of next generation optical devices. To investigate the optical properties of TCOs at nanoscale, in this thesis, several new kinds of colloidal nanocrystals (NCs) of TCOs have been synthesized and their optical emission and transparency have been explored. The first part of my work focuses on ITO (indium tin oxide) NCs demonstrates phase and size dependence of surface plasmon absorption in the near infrared region. The second part of the thesis describes colloidal synthesis of γ-Ga2O3 with size tunable photoluminescence, further study reveals that the photoluminescence is defect related and can be tuned by changing the defect concentration. In the last part of my study, I develop a methodology for lanthanide doped γ-phase Ga2O3 NCs and reveal tunable chromaticity of the lanthanide doped NCs.

Transparent conducting oxides (TCOs) usually have high conductivity and transparency in the visible range and have been widely used in daily life. Recently, TCOs have attracted great interest due to their potential applications in various new optical and electrical devices (flat-panel displays, energy efficient windows, etc.). Nanostructured TCOs can induce new size related properties, for example, when sizes of TCOs are controlled at the nanometer scale, various defects can introduce different defect-related optical emissions. These new nanostructured TCOs combining traditional and new size dependent properties may be used for construction of next generation optical devices. To investigate the optical properties of TCOs at nanoscale, in this thesis, several new kinds of colloidal nanocrystals (NCs) of TCOs have been synthesized and their optical emission and transparency have been explored. The first part of my work focuses on ITO (indium tin oxide) NCs demonstrates phase and size dependence of surface plasmon absorption in the near infrared region. The second part of the thesis describes colloidal synthesis of γ-Ga2O3 with size tunable photoluminescence, further study reveals that the photoluminescence is defect related and can be tuned by changing the defect concentration. In the last part of my study, I develop a methodology for lanthanide doped γ-phase Ga2O3 NCs and reveal tunable chromaticity of the lanthanide doped NCs.

Geopolymers, a class of largely X-ray amorphous aluminosilicate binder materials, have been studied extensively over the past several decades, but largely from an empirical standpoint. The primary aim of this investigation has been to apply a more science-based approach to the study of geopolymers, including introducing a variety of mathematical modelling techniques to the field. The nanostructure of geopolymers is analysed via an extensive literature review, and conclusions regarding the presence and role of crystallinity within the geopolymer structure are drawn. Si/Al ordering within the tetrahedral aluminosilicate gel framework is described by a statistical thermodynamic model, which provides an accurate representation of the distribution of Si and Al sites within the framework as well as physically reasonable values for the energy penalty associated with ordering violation. Framework and extraframework structure within the geopolymer binder are also described by the pair distribution function (PDF) technique, whereby synchrotron X-ray scattering data are converted via a Fourier transform-based method into real-space structural data on an Ångstrom length scale. Real-space Rietveld analysis of geopolymers crystallised at high temperature is used to back-calculate and analyse the original geopolymer structure, and the primary change in very short-range structure from the as-synthesised geopolymer to the high-temperature crystalline product is observed to be a shift in the location of the extraframework charge-balancing cation.

Low dimensional semiconductors are promising materials with diverse range of applications in a variety of fields. Specifically, in recent times low dimensional oxide and sulfide based semiconductors are regarded as materials that can have potential applications in chemical gas sensor, optoelectronic devices and memristor. How ever, in some cases it is envisioned that appropriate doping as well as phase stabilization is important in enhancing their material properties. This work presents the synthesis, characterization and application of various (pristine and doped) quasi-one dimensional metal oxides (TiO2, VO2) and two-dimensional materials (CuO thin film, MoS2). Some practical protocols for stabilization of specific phases at ambient conditions via a new method of doping in VO2 nanostructures with aluminum, is demonstrated. Similarly, a temperature-doping level phase diagram for the free-standing nanostructures in the temperature range close to the ambient conditions was presented. TiO2 nanowire was doped during growth and electrical measurements on individual TiO2 single crystal nanowires indicate that light in visible range can induce electron-hole pair formation. Furthermore, gas sensing (CO, H2) measurements taken under visible light irradiation imply that photo-activated chemical oxidization on the surface of TiO2 nanowires occurs, which is responsible for the observed measurements. Further, the effect of self heating in some nanostructures was also explored. Since self-heating is a prospective power-efficient energy delivery channel to the conductometric chemical sensors that require elevated temperatures for their operation, the unprecedentedly low power consumption can be achieved via minimizing the heat dissipation in the optimized device architecture. By investigating the heat dissipation in these devices we show that the thermal, electrical and chemical properties of the self-heated semiconducting nanowires appear to be strongly coupled with each other at nanoscale. This opens up unique opportunity to fabricate low power nanoscopic sensing leading to an ultra-small and power efficient single nanostructure gas recognition system. The CuO film based lateral devices were fabricated and studied for its resistive switching behavior. A good, stable and reproducible threshold RS performance of CuO film was obtained by electrical measurement. Finally, the micro-flake MoS2 based FET photoelectronic device was fabricated (using mechanically exfoliated MoS2) and its electronic and photoelectronic properties were investigated. We show that though the FET mobility values of MoS2 microflake is in the average range, but the photo-responsivity is much higher compared to most of others similar sulfide based 2D layered materials.

abstract: In this thesis, a novel silica nanosphere (SNS) lithography technique has been developed to offer a fast, cost-effective, and large area applicable nano-lithography approach. The SNS can be easily deposited with a simple spin-coating process after introducing a N,N-dimethyl-formamide (DMF) solvent which can produce a highly close packed SNS monolayer over large silicon (Si) surface area, since DMF offers greatly improved wetting, capillary and convective forces in addition to slow solvent evaporation rate. Since the period and dimension of the surface pattern can be conveniently changed and controlled by introducing a desired size of SNS, and additional SNS size reduction with dry etching process, using SNS for lithography provides a highly effective nano-lithography approach for periodically arrayed nano-/micro-scale surface patterns with a desired dimension and period. Various Si nanostructures (i.e., nanopillar, nanotip, inverted pyramid, nanohole) are successfully fabricated with the SNS nano-lithography technique by using different etching technique like anisotropic alkaline solution (i.e., KOH) etching, reactive-ion etching (RIE), and metal-assisted chemical etching (MaCE). In this research, computational optical modeling is also introduced to design the Si nanostructure, specifically nanopillars (NPs) with a desired period and dimension. The optical properties of Si NP are calculated with two different optical modeling techniques, which are the rigorous coupled wave analysis (RCWA) and finite-difference time-domain (FDTD) methods. By using these two different optical modeling techniques, the optical properties of Si NPs with different periods and dimensions have been investigated to design ideal Si NP which can be potentially used for thin c-Si solar cell applications. From the results of the computational and experimental work, it was observed that low aspect ratio Si NPs fabricated in a periodic hexagonal array can provide highly enhanced light absorption for the target spectral range (600 ~ 1100nm), which is attributed to (1) the effective confinement of resonant scattering within the Si NP and (2) increased high order diffraction of transmitted light providing an extended absorption length. From the research, therefore, it is successfully demonstrated that the nano-fabrication process with SNS lithography can offer enhanced lithographical accuracy to fabricate desired Si nanostructures which can realize enhanced light absorption for thin Si solar cell. / Dissertation/Thesis / Doctoral Dissertation Materials Science and Engineering 2015