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UBC Theses and Dissertations

ZnO-based thermoelectrics : modelling, electrochemical thick film growth, and characterization Sielmann, Christoph


The thermoelectric performance of electrodeposited, aluminum doped zinc oxide was assessed. In this work, wurtzite ZnO was first modelled using Mueller-Plathe to compare the effectiveness of different nanostructured configurations on reducing thermal conductivity. A new analysis technique, Local Vibrational Density of States Equilibrium Molecular Dynamics (LVDOS-EMD), was created to study localized lattice vibrations around nanostructural features of silicon and ZnO, and was used to predict thermal properties in materials of similar composition 17× faster than conventional thermal modelling methods. A 30% void density was determined to yield the best reduction in thermal conductivity by volume of voids in bulk Al:ZnO with a computed thermal conductivity of 0.77 W m-¹ K-¹ at room temperature, 3× below the threshold achieved through established experimental means with high electrical conductivity Al:ZnO. Thick film, electrodeposited Al:ZnO was grown using a nitrate system. Experiments on solution pH using various counter electrodes demonstrated that inert electrodes caused acidification of the growth solution, limiting film thickness. Chloride contamination from commonly used Ag/AgCl reference electrodes was also determined to affect thick film opacity, morphology, crystallinity, and electrical properties. Aluminum integration and activation was explored by adding Al(NO₃)₃ to the growth solution during film synthesis, yielding aluminum integration molar ratios of up to 1.72% (Al.₀₃₄Zn.₉₆₆₀). Partially doped films in excess of 95 µm thick, 4× the thickness reported elsewhere, were electrochemically grown and characterized. Sub-micron voids were integrated into the films using sacrificial material and annealing. A new electrochemical chromium etching methodology was developed and successfully used to free 20 films from their growth substrates for thermoelectric characterization. A new, reusable thermoelectric test apparatus for thin film thermoelectric testing was designed, implemented, calibrated, and successfully deployed to characterize ZnO and Al:ZnO thin films grown 79 – 95 µm in thickness. Extremely low thermal conductivity of 11 mW m-¹ K-¹ at room temperature was demonstrated concurrently with a Seebeck coefficient of -88 µV K-¹. Polycrystallinity and poor dopant activation yielded a low electrical conductivity of 0.75 mS/cm and corresponding low room temperature ZT of 1.3×10-⁵ for the Al:ZnO films.

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