Since the discovery of organic semiconductors (OSCs) over four decades ago, the field of organic electronics has broken our misconceptions regarding the possibilities of modern electronics. The synthetic toolkit of organic chemistry enables the creation of a limitless number of unique OSCs that can be specifically tailored and engineered with the specific and desired properties for unique applications. The rapid adoption of modern information systems, “Internet of Things,” in which smart devices and sensors ubiquitously collect and exchange data has resulted in a need for low-cost sensors to be deployed everywhere from the monitoring of food supply chains, environmental conditions, to human health. Organic thin-film transistors (OTFTs) are a necessary component to support these technologies. However, their mass adoption will require reduction in cost and improved compatibility with low voltage generating printed batteries or flexible and ultrathin photovoltaics. This thesis is focused on the development of high performing solid state polymer electrolytes to be employed as the gating medium in OTFTs. The choice of conventional gating materials often leads to a tradeoff between high capacitance, operating speed and material softness. For example liquid electrolyte gating materials have high capacitance but low operating speed and are liquid at room temperature which is unacceptable for many electronics application. Polymer gating materials often have lower capacitance but fast operating conditions and solid at room temperature. In this thesis we establish structure property relationships which aid in the design of novel block copolymer-based gating materials which simultaneously enable the increase in capacitance and switching speed while remaining solid at room temperature. In the first study I established a styrene-based ionic liquid monomer can be using as a controlling monomer in the nitroxide mediated copolymerization of methacrylates. The second study then focuses on the integration of these materials into OTFT devices; the morphology (block vs random copolymers) effect on device performance is assessed. The last study builds on the findings of the previous study and further explores the structural elements of block copolymers on device performance. The work presented here outlines the development of advanced poly(ionic liquid) based solid electrolyte materials that enables both reduced operating voltages and fast switching. Finally, we establish structure-property relationships that relate the molecular architecture to OTFT device performance paving the way for the adoption of a new generation of high performing, printable and flexible electronics.

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Increasing demand for high-density memories has necessitated the search for new materials with higher dielectric constants to satisfy the minimum charge storage density requirements. Several materials such as Ta₂O₅, BST¹, BBT² are being investigated to replace the currently used Si based oxide/nitride dielectrics. Among the materials under investigation, Ta₂O₅ is one of the most promising, especially from the fab compatibility point of view. Ta₂O₅ thin films offer a six-fold increase in dielectric constant compared to conventional dielectrics. However, the significant improvement in dielectric constant is offset by higher leakage currents compared to conventional dielectrics. Improvement in both, dielectric and insulating properties is required for the successful integration of Ta₂O₅ thin films into devices. In the current research work, it was demonstrated that by chemically modifying the tantalum pentoxide matrix, significant improvements in its electrical properties can be achieved which would enable the fabrication of a reliable high-density memory device. In the present work, the effects of Al addition on Ta₂O₅ thin films were systematically studied. The structural and electrical properties of these chemically modified thin films were investigated in detail to establish their potential for device applications. The effects on dielectric and insulating characteristics due to incorporation of Al in Ta₂O₅ matrix were studied in capacitor configuration. A metallorganic solution decomposition (MOSD) technique was used to deposit thin films onto Pt coated Si(100) substrates. The capacitors were fabricated by sputter depositing Pt electrodes on the top surface of the films. The dielectric and insulating properties of pure and modified Ta₂O₅ thin films and their dependence on film composition, processing temperature, and the thickness were discussed and an attempt was made to provide theoretical understanding for the experimental observations. The dielectric and insulating properties of Ta₂O₅ were found to be significantly modified by addition of Al. It was observed that Al addition has decreased the leakage currents approximately by an order of magnitude and improved thermal and bias stability characteristics of Ta₂O₅ capacitors. For example, the leakage currents in crystalline pure Ta₂O₅ thin films were found to be 4.5 x 10⁷ A/cm² in a 1MV/cm dc field which decreased to 3.4 x 10⁸ A/cm² for 10% Al modified Ta₂O₅ thin films. A typical dielectric constant of 42.5 was obtained for 10% Al modified Ta₂O₅ thin films. This is significantly higher compared to the commonly reported dielectric constant of 25 to 35 for Ta₂O₅ thin films. This enhancement was attributed to strong (100) orientation exhibited by both pure and modified Ta₂O₅ thin films. The high dielectric constant, low dielectric loss, low leakage currents and low temperature coefficient of capacitance suggest the suitability of Al modified Ta₂O₅ as a capacitor dielectric for future generation DRAM applications. ¹Barium strontium titanate, ²Barium bismuth tantalate / Master of Science

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The development and implementation of biosensors as an integral and growing part of our modern world has prompted the push for precision health as the next step in medicine. Adapted from aircraft engine monitoring, where an array of sensors is used to build a digital twin to preemptively predict problems, precision health requires an increase in molecular monitoring. Organic thin-film transistors (OTFTs), as sensitive, low-cost, and adaptable devices are well suited to meet this need. Phthalocyanines (Pcs), as an organic semiconducting layer for OTFTs, are easily synthesized and highly tunable small molecules which can be deposited through both solution and physical vapor deposition techniques, enhancing their utility. This work presents Pc-based OTFTs for cannabinoid sensing and chemotyping to meet the quality control needs of a growing Canadian and International cannabis industry, and to broadly demonstrate the sensitivity and selectivity attainable with Pc-based OTFTs incorporating molecular analyte sensors. Spectroelectrochemistry is established as a screening technique for Pc-based OTFT sensors and, in combination with thin-film characterization, is used to propose a mechanism for Pc-cannabinoid interactions and OTFT cannabinoid sensitivity with and without a cannabinoid-sensitive chromophore. Thin-film morphologies and polymorphs, pre- and post-analyte exposure, are demonstrated as key drivers of Pc-based OTFT sensing responses and are further explored through controlled deposition conditions and post deposition annealing techniques. Through material screening and thin-film engineering, part-per-billion cannabinoid sensitivity is achieved with Pc-based OTFTs. This report documents several strategies for sensitizing Pc-based OTFT sensors to organic analytes, and the results herein serve as a basis for continued development of Pc-based OTFT biosensors.

<p> Tantalum thin film resistors have been reactively sputtered in oxygen and nitrogen simultaneously. The films studied had resistivities ranging from 400μΩ-cm to 3 x 10^4 μΩ-cm. The corresponding TCR values ranged from -50 ppm/°C to -2,000 ppm/°C. Conductance-temperature measurements show that electrical conduction in discontinuous films of metallic islands (typically 100 A°) largely surrounded by regions of Ta2O5 (typically 50 A°) may be due to a tunneling mechanism of negative TCR operating concurrently with a metallic mechanism of positive TCR via interconnected metallic islands.</p> <p> Irradiation of these discontinuous films by 150 keV protons produces a conductance increase which is attributed to an enhanced tunneling mechanism via electronic defect levels in the inter-island oxide regions. During irradiation of these films at 30°K, the conductance change increases and approaches apparent saturation. This nonlinearity is attributed to a combination of spontaneous recombination and close-pair thermal annealing. The number of unstable sites surrounding each defect is found to be ≥ 4. Thermal recovery of the conductance proceeds in two main stages: Stage A (34°K to 150°K) is attributed to close-pair or correlated recombination; Stage B (150°K to 300°K) is attributed to uncorrelated migration of defects to gap-island interfaces, as is indicated by the greatly reduced Stage B annealing which is observed for continuous, polycrystalline films of Ta2O5, having a typical grain size of 1,500 A°. Negative annealing stages (characterized by a conductance increase) indicate a metallic conduction process via connected metallic islands.</p> <p> For 286°K irradiation of discontinuous films, the conductance initially increases with fluence in a nonlinear fashion until a threshold fluence is reached, at which point the conductance decreases with fluence. The nonlinearity of the conductance increase is attributed to trapping of mobile radiation-produced defects at gap-island interfaces during irradiation. The subsequent conductance decrease is attributed to a shift in the Fermi level, and thus the height of the tunneling barrier, as the result of the formation of unequal concentrations of stable radiation-produced donor and aeceptor defects since unequal concentrations of these defects can be expected to annihilate at the gap-island interface. The absence of this conductance decrease in continuous polycrystalline films is consistent with this model, since the absence of gap-island interfaces is expected to result in equal concentrations of stable donor and acceptor levels being produced.</p> <p> The observed negative increase in TCR with fluence is attributed to an increase in the proportion of the tunneling mechanism of negative TCR (as the result of radiation-produced defects in the inter-island oxide regions) relative to the proportion of the metallic conduction mechanism of positive TCR. The difference between the TCR recovery after irradiation at 30°K (little recovery between 150°K and 300°K) and the conductance recovery (about 50 percent of the recovery occurs between 150°K and 300°K) is attributed to the expected greater influence of metallic recovery on the annealing of the film TCR relative to the annealing of the film conductance.</p> / Thesis / Doctor of Philosophy (PhD)

Thesis / Master of Engineering (MEngr)

<p> As part of a CdS-cu2s thin film solar cell research project, a CdS evaporation system was designed and built using an Edwards 19E6 coating unit. With the overall aims of the project in mind, the apparatus was designed as part of a CdS-Cu2s dual, in situ, evaporation system. CdS films, ranging in thickness from lμ to 25μ, produced by this system, were characterized optically, electrically and crystallographically as functions of the various evaporation parameters. </p> / Thesis / Master of Engineering (MEngr)

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