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This thesis studies parameters influencing both the performance and stability of solid state sensitized solar cells (ssSSCs). ssSSCs benefit from their low materials and manufacturing processing costs, a consequence of using solution processed materials. However, solution processed materials are often structurally and electronically disordered. By characterizing fully operational ssSSCs and their charge transport properties, this thesis elucidates the factors limiting charge transport and proposes routes towards both improved photovoltaic conversion efficiency and long-term stability. Chapter 2 provides an explanation of the operation of ssSSCs, while Chapter 3 discusses the basic methods used in this thesis. Having set this background, Chapter 4 explores the interaction between atmospheric oxygen and charge doping mechanisms in the organic semiconductors used in ssSSCs. To understand the implications of the findings presented in Chapter 4, a new technique, “transient mobility spectroscopy”, was developed to understand the evolution of balanced charge transport behaviour of disordered semiconductors at different operating conditions in ssSSCs. This technique is presented in full in Chapter 5. The understanding gained in Chapters 4 and 5 suggest that alternative light absorbers with higher extinction coefficients may be beneficial to improving the performance of ssSSCs. Chapter 6 discusses the use of an organometal trihalide perovskite, as light absorber in ssSSCs. Using time resolved techniques, the charge transport and recombination mechanisms in various device architectures are explored, allowing suggestions to be made towards future improvements. Chapter 7 uses the technique presented in Chapter 5 to understand a rapid degradation mechanism of working ssSSCs. Particular focus is placed on the titanium dioxide charge-transporting layer. Building on this newfound understanding, two methods for attaining stable photovoltaic performance are provided, a great step forward for this technology.

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Novel methods for the construction of dye-sensitized solar cells (DSSCs) were developed. A thin dense underlayer of TiO2 was applied on fluorine-doped tin oxide (FTO) glass using as a precursor Tyzor AA-105. Subsequently a mesoporous film of P-25 TiO2 was applied by spreading a suspension uniformly over the surface of the underlayer and allowing the plate to slowly dry while resting on a level surface. After sintering at 500° C slides were treated with TCPP as a sensitizing dye and assembled into DSSCs. A novel method was used to seal the cells; strips of Parafilm® were used as spacers between the electrodes and to secure the electrodes together. The cells were filled with a redox electrolyte and sealed by dipping into molten paraffin. A series of phosphonic acids and one arsonic acid were employed as coadsorbates in DSSCs. The coadsorbates were found to compete for binding sites, resulting in lower levels of dye adsorption. The resulting loss of photocurrent was not linear with the reduction of dye loading, and in some cases photocurrent and efficiency were higher for cells with lower levels of dye loading. Electrodes were treated with coadsorbates by procedures including pre-adsorption, simultaneous (sim-adsorption), and post-adsorption, using a range of concentrations and treatment times and a variety of solvents. Most cells were tested using an iodide-triiodide based electrolyte (I3I-1) but some cells were tested using electrolytes based on a Co(II)/Co(III) redox couple (CoBpy electrolytes). Phosphonic acid post-adsorbates increased the Voc of cells using CoBpy electrolytes but caused a decrease in the Voc of cells using I3I-1 electrolyte. Phosphonic acids as sim-adsorbates resulted in a significant increase in efficiency and Jsc, and they show promise as a treatment for TCPP DSSCs.

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Thin-film solar cells are widely recognised to have the potential to compete with fossil fuels in the electricity market due to their low cost per peak Watt. The Thin-Film Group at the University of New South Wales (UNSW) is engaged in developing polycrystalline silicon (poly-Si) thin-film solar cells on glass using e-beam evaporation technology. We believe our solar cells have the potential of significantly lowering the manufacturing cost compared to conventional, PECVD-fabricated thin-film solar cells. After years of materials research, the focus of the Group??s work is now moving to the metallisation of evaporated solar cells. Minimising various kinds of losses is the main challenge of the cell metallisation procedure, within which the contact resistance is always a big issue. In this thesis, the contact resistance of aluminium contacts on poly-Si thin-film solar cells on glass is investigated. To the best of the author??s knowledge, this is the first ever contact resistance investigation of Al contacts on evaporated poly-Si material for photovoltaic applications. Various transmission line models (TLM) are employed to measure the contact resistance. An improved TLM model is developed to increase the measurement precision and, simultaneously, to simplify the TLM pattern fabrication process. In order to accommodate the particular requirements of poly-Si coated glass substrates, a TLM pattern fabrication process using photolithography is established. Furthermore, a Kelvin sense tester is set up to ensure an accurate measurement of the contact resistance. After establishment of the TLM technique at UNSW, it is successfully tested on singlecrystalline silicon wafer samples. The thermal annealing process of the contacts is also optimised. Then, the general behaviour of Al contacts on uniformly doped poly-Si films (i.e., no p-n junction) is investigated using the verified TLM technique. The long-term stability of the contacts is also studied. This is followed by an investigation of the contact resistance of the back surface field and emitter layers of different types of poly-Si thin-film solar cells. Finally, a novel contact resistance measurement model is proposed that is believed to be able to overcome the measurement bottleneck of the transmission line models.

Solar energy is the foremost power source of our planet. Driving photosynthesis on our planet for 3 billion years the energy stored in the form of fossil fuels also originates from the sun. Consumption of fossil fuels to generate energy is accompanied with CO2 emission which affects the earth's climate in a serious manner. Therefore, alternative ways of converting energy have to be found. Solar cells convert sunlight directly into electricity and are therefore an important technology for future electricity generation. In this work solar cells based on the inorganic semiconductor titanium dioxide and hole-transporting dyes are investigated. These type of solar cells are categorized as hybrid solar cells and are conceptually related to both dye-sensitized solar cells and organic solar cells. Light absorption in the bulk of the hole-transporting dye layer leads to the formation of excitons that can be harvested at the organic/inorganic interface. Two design approaches were investigated: 1) utilizing a multilayer of a hole-transporting dye and 2) utilizing a hole-transporting dye as light harvesting antenna to another dye which is bound to the titanium dioxide surface.  Using a multiple dye layer in titanium dioxide/hole transporting dye devices, leads to an improved device performance as light harvested in the consecutive dye layers can contribute to the photocurrent. In devices using both an inteface-bound dye and a hole-transporting dye, excitation energy can be transferred from the hole-transporting dye to the interface dye.

Organic materials, such as conjugated polymers, have emerged as a promising alternative for the production of inexpensive and flexible photovoltaic cells. As conjugated polymers are soluble, liquid based printing techniques enable production on large scale to a price much lower than that for inorganic based solar cells. Present day state of the art conjugated polymer photovoltaic cells are comprised by blends of a semiconducting polymer and a soluble derivative of fullerene molecules. Such bulk heterojunction solar cells now show power conversion efficiencies of up to 4-6%. The quantum efficiency of thin film organic solar cells is however still limited by several processes, of which the most prominent limitations are the comparatively low mobility and the high level of charge recombination. Hence organic cells do not yet perform as well as their more expensive inorganic counterparts. In order to overcome this present drawback of conjugated polymer photovoltaics, efforts are continuously devoted to developing materials or devices with increased absorption or with better charge carrier transporting properties. The latter can be facilitated by increasing the mobility of the pure material or by introducing beneficial morphology to prevent carrier recombination. Minimizing the active layer film thickness is an alternative route to collect more of the generated free charge carriers. However, a minimum film thickness is always required for sufficient photon absorption. A further limitation for low cost large scale production has been the dependence on expensive transparent electrodes such as indium tin oxide. The development of cheaper electrodes compatible with fast processing is therefore of high importance. The primary aim of this work has been to increase the absorption in solar cells made from thin films of organic materials. Device construction, deploying new geometries, and evaluation of different methods to provide for light trapping and photon recycling have been strived for. Different routes to construct and incorporate light trapping structures that enable higher photon absorption in a thinner film are presented. By recycling the reflected photons and enhancing the optical path length within a thinner cell, the absorption rate, as well as the collection of more charge carriers, is provided for. Attempts have been performed by utilizing a range of different structures with feature sizes ranging from nanometers up to centimeters. Surface plasmons, Lambertian scatterers, micro lenses, tandem cells as well as larger folded cell structures have been evaluated. Naturally, some of these methods have turned out to be more successful than others. From this work it can nevertheless be concluded that proper light trapping, in thin films of organic materials for photovoltaic energy conversion, is a technique capable of improving the cell performance. In addition to the study of light trapping, two new alternative electrodes for polymer photovoltaic devices are suggested and evaluated.

In this work, spin-on processes were used to improve front- and rear-side technologies of solar cells to increase efficiencies to >20 %. A limited source diffusion process was developed using phosphoric acid dopant solutions developed in-house. An optimal emitter was obtained to be used in conjunction with screen-printed contacts. This emitter was used to improve the efficiency of conventional full aluminum back surface field solar cells to 19.6 %. A streamlined process was then developed to fabricate high-efficiency dielectric rear passivated cells in a single high temperature step. This process combined the diffusion process described earlier with a spin-on dielectric for rear passivation to achieve solar cell efficiencies of ~20%. Several laser candidates were investigated to improve process reproducibility and throughput. Ultra-violet laser with nanosecond pulse width was identified as the optimal choice. Cell efficiencies of ~20% were reproduced using UV laser for ablation of rear dielectric. This cell design and process were transferred to low-cost low-lifetime commercial grade substrates after identifying the optimal substrate characteristics using modeling.