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Organic electrode materials, as sustainable and environmental benign alternatives to inorganic electrode materials, show great promise for achieving cheap, light, versatile and disposable devices for electrical energy storage applications. Conducting redox polymers (CRPs) are a new class of organic electrode materials where the charge storage capacity is provided by the redox chemistry of functional pendent groups and electronic conductivity is provided by the doped conducting polymer backbone, enabling the production of energy storage devices with high charge storage capacity and high power capability. This pendant-conducting polymer backbone combination can solve two of the main problems associated with organic molecule-based electrode materials, i.e. the dissolution of the active material and the sluggish charge transport within the material. In this thesis, diethyl terephthalate and polythiophenes were utilized as the pendant and the backbone, respectively. The choice of pendant-conducting polymer backbone combination was based on potential match between the two moieties, i.e. the redox reaction of terephthalate pendent groups and the n-doping of polythiophene backbone occur in the same potential region. The resulting CRPs exhibited fast charge transport within the polymer films and low activation energies involved charge propagation through these materials. In the design of these CRPs an unconjugated link between the pendant and the backbone was found to be advantageous in terms of the polymerizability of the monomers and for the preservation of individual redox activity of the pendants and the polymer chain in CRPs. The functionalized materials were specifically designed as anode materials for energy storage applications and, although insufficient cycling stability was observed, the work presented in this thesis demonstrates that the combination of redox active functional groups with conducting polymers, forming CRPs, shows promise for the development of organic matter-based electrical energy storage materials.

Recent work has proposed sliders as a useful way to measure self-reported emotion continuously. My dissertation extends this work to ask: what are relevant properties of affective self-report on sliders and variations? How reliable are affective self-reports? How do they relate to physiological data? What are individual and cultural differences? How can this method be applied to ehealth? Three emotion self-report tools (one-slider, two-slider, a touchscreen) were developed and evaluated in four experiments. The first experiment was within-subjects. Participants viewed short videos, with four self-report conditions (including no reporting) and physiological capture (heart rate variability and skin conductance). In a re-rating task, the sliders models were found to be more reliable than the touchscreen (Lottridge & Chignell, 2009a). The second and third experiments were between-subjects, and examined individual and cultural differences. Canadian and Japanese participants watched a nature video, while rating emotions and answering questions. Analyses were carried out within and across the datasets. Larger operation span displayed a minor benefit. Valence and arousal ratings were not strongly related to skin conductance. The Japanese performed on par with Canadians but reported worse performance. Based on the results, the recommendation was made that a single slider be used to rate valence, that arousal be estimated with skin conductance, and that slider psychometrics be used to assess cognitive load over time. In the fourth experiment, diabetic participants watched Diabetes-related videos. They clustered into usage patterns: some moved the slider very little during videos and more afterward, some hardly moved the slider, and some used it as expected. Two novel metrics facilitated these analyses: Emotional Bandwidth, an application of information entropy that characterizes the granularity of the self reports (Lottridge & Chignell, 2009b) and Emotional Majority Agreement, the amount of agreement relative to a sample’s self-reports (Lottridge & Chignell, 2009c). In summary, this dissertation contributes a method of measuring emotion through sliders and skin conductance that has been evaluated in a number of experimental studies. It contributes the empirical results, design recommendations, and two novel metrics of emotional response. Limitations and implications for future research and practice are also discussed.

Recent work has proposed sliders as a useful way to measure self-reported emotion continuously. My dissertation extends this work to ask: what are relevant properties of affective self-report on sliders and variations? How reliable are affective self-reports? How do they relate to physiological data? What are individual and cultural differences? How can this method be applied to ehealth? Three emotion self-report tools (one-slider, two-slider, a touchscreen) were developed and evaluated in four experiments. The first experiment was within-subjects. Participants viewed short videos, with four self-report conditions (including no reporting) and physiological capture (heart rate variability and skin conductance). In a re-rating task, the sliders models were found to be more reliable than the touchscreen (Lottridge & Chignell, 2009a). The second and third experiments were between-subjects, and examined individual and cultural differences. Canadian and Japanese participants watched a nature video, while rating emotions and answering questions. Analyses were carried out within and across the datasets. Larger operation span displayed a minor benefit. Valence and arousal ratings were not strongly related to skin conductance. The Japanese performed on par with Canadians but reported worse performance. Based on the results, the recommendation was made that a single slider be used to rate valence, that arousal be estimated with skin conductance, and that slider psychometrics be used to assess cognitive load over time. In the fourth experiment, diabetic participants watched Diabetes-related videos. They clustered into usage patterns: some moved the slider very little during videos and more afterward, some hardly moved the slider, and some used it as expected. Two novel metrics facilitated these analyses: Emotional Bandwidth, an application of information entropy that characterizes the granularity of the self reports (Lottridge & Chignell, 2009b) and Emotional Majority Agreement, the amount of agreement relative to a sample’s self-reports (Lottridge & Chignell, 2009c). In summary, this dissertation contributes a method of measuring emotion through sliders and skin conductance that has been evaluated in a number of experimental studies. It contributes the empirical results, design recommendations, and two novel metrics of emotional response. Limitations and implications for future research and practice are also discussed.

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Mémoire numérisé par la Direction des bibliothèques de l'Université de Montréal.

<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)

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