published_or_final_version / Physics / Doctoral / Doctor of Philosophy

There has been an increased interest in renewable energy systems in recent years as a result of concerns on depleting fossil fuel reserves and climate change. Wind and solar energy are amongst the most popular renewable energy technologies. In order to use the full or maximum possible extent of a renewable energy resource in a region, hybrid systems extracting wind and solar energy simultaneously are a popular and obvious choice. It is desired to design hybrid systems that enhance the renewable energy output without increasing the foot print area compared to the base case of only wind or only solar energy. One potential way forward is to consider a vertical axis wind turbine with an enhanced surface area which can be used for mounting solar cells. This way the foot print area remains the same while both wind and solar power are obtained simultaneously. Renewable Energy Solutions LLC has manufactured a novel 2 m high and 2 m in diameter vertical axis wind turbine called Marilyn which has an enhanced surface area, which can be used for the aforementioned purpose. This thesis focuses on the development of a hybrid solar-wind turbine design based on the Marilyn system. Firstly, the wind and solar resource was assessed at Austin, TX using weather monitoring instruments. Typical Meteorological Year 3 (TMY3) data was also used in conjunction with the measured data to estimate the wind and solar resource at Austin, TX. Secondly, the wind turbine performance was assessed based on whether is it able to achieve grid tie in for wind power production starting at wind speeds of 3-4 m/s. It was found that replacing the current generator with different model featuring higher voltage output at lower rotational speeds could help achieve this. Based on this suggested replacement and using the wind resource data, the yearly wind energy production was estimated to be 240 kWh. Finally, a theoretical analysis was performed for estimating the yearly solar energy production. A base case analysis was first made on power production on a particular day of the year if only the top portion of every alternate face of the turbine is covered with flexible 3.4 % efficient solar cells. This analysis is subsequently extended to the case when flexible 20 % efficient solar cells cover the entire top surface of the turbine and the corresponding conservative yearly solar energy output was estimated to be 310 kWh. Thus the total yearly energy output from the Marilyn hybrid system is 550 kWh, which is around 5 % of the annual electricity usage of a typical American home / text

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The main goal of this thesis is to investigate and develop the physics of dye-based photovoltaic physics through molecular and photonic routes. Numerous photovoltaics devices have been fabricated through the course of this work to study their characteristics, performance, physical composition and action. The relative youth of the field of dye-based optoelectronics provides extensive scope for new research which provides fascinating opportunities in terms of physical processes.This thesis is divided into two main projects; exploring the adaption of conventional dye-sensitized solar cells via starkly different routes which serendipitously culminated in striking similarities at their conclusion. The first route is through incorporating spectrally complementary dye molecules with the intention of extending the range of light absorption of the final devices. This initial aim was achieved and was then furthered by the realisation of an unexpected and unprecedented energy transfer process occurring, imparting enhanced photocurrent generation in both the near-IR and visibile region. The second route involves investigating the effect on dye-sensitized solar cell physics and performance of the inclusion of metallic nanoparticles with the expectation of inducing plasmonic interactions. Novel systems were designed and implemented, devices were made which display significant performance enhancement, attributed to plasmonic coupling into the dyes and thereby increasing photocapture. A number of other investigations are documented whose current completion does not sufficiently warrant independent chapters but whose scientific interest is evident.

This thesis describes the synthesis of a novel family of porphyrins fused to anthracenes, together with investigations into their optical and electrochemical properties, as well as exploring their potential for application in dye-sensitised solar cells. Chapter 1 gives an overview of the structure-property relationships of large planar pi- systems for organic electronic applications. Porphyrins are introduced as suitable building blocks for such systems, and approaches for extending the pi-conjugation of these macrocycles are presented. A literature review of porphyrins fused to aromatic units is presented in Chapter 2, with a focus on the influence of structure on the optoelectronic properties of such systems. The chapter concludes with a summary of my previous work on the synthesis of anthracene-fused porphyrins, and the aims of this project are stated. Chapter 3 describes the syntheses of fully and partially fused bis-anthracene porphyrin monomers and dimers. By varying peripheral substituents, it was possible to solve problems of aggregation encountered for these systems. Fusion of anthracene units to a porphyrin core was found to result in systems displaying strong absorption in the near-IR, small HOMO-LUMO gaps, and low oxidation potentials. Chapter 4 explores the synthesis, crystal structure and optoelectronic properties of a porphyrin fused to four anthracenes, revealing this system to exhibit the longest wavelength absorption of any porphyrin monomer. The synthesis of a liquid crystalline tetra-anthracene-fused porphyrin was proposed, and attempts to synthesise the necessary anthracene precursors were undertaken. Chapter 5 describes the molecular design and synthetic pathway to a mono-anthracene fused porphyrin, and its unfused analogue, for use in liquid electrolyte dye-sensitised solar cells. By varying the metal oxide layer or lithium ion concentration of the device, it was possible to achieve incident photon to current conversion efficiency (IPCE) responses at wavelengths beyond 1050 nm. Chapter 6 details the experimental synthetic procedures and characterisation data for all the compounds synthesised during this project.

A genetic algorithm was used to optimize the power output of multi-junction solar cells. Solar cell operation was modeled using the Silvaco ATLASTM software. The output of the ATLASTM simulation runs served as the input to the genetic algorithm. The genetic algorithm was run as a diffusing computation on a network of eighteen dual processor nodes. Results showed that the genetic algorithm produced better power output optimizations when compared with the results obtained using the hill climbing/gradient approach.

Recent advances in third generation photovoltaics, particularly the rapid increase in perovskite power conversion efficiencies, may provide a cheap alternative to silicon solar cells in the near future. A key component to these devices is the transparent front electrode, and in the case of Dye Sensitized Solar Cells, it is the most expensive part. A lightweight, cost-effective, robust, and easy-to-fabricate new generation TCE is required to enable competition with silicon. Indium Tin Oxide, commonly used in touchscreen devices, Organic Light Emitting Diodes (OLEDs), and thin film photovoltaics, is widely used and commonly referred to as the industry standard. As the global supply of indium decreases and the demand for this TCE increases, a similar alternative TCE is required to accompany the next generation solar cells that promise energy with lighter and significantly cheaper modules. This alternative TCE needs to provide similar sheet resistance and optical transmittance to ITO, while also being mechanically and chemically robust. The work in this thesis begins with an exploration of several synthesized ITO replacement materials, such as copper nanowires, conductive polymer PEDOT:PSS, zinc oxide thin films, reduced graphene oxide and combinations of the above. A guiding philosophy to this work was prioritizing cheap, easy deposition methods and overall scalability. Shortcomings of these TCEs were investigated and different materials were hybridized to take advantage of each layers strengths for development of an ideal ITO replacement. For CuNW-based composite electrodes, ~85% optical transmittance and ~25 Ω/sq were observed and characterized to understand the underlying mechanisms for optimization. The second half of this work is an examination of many different perovskite synthesis methods first to achieve highest performance, and then to integrate compatible methods with our CuNW TCEs. Several literature methods investigated were irreproducible, and those that were successful posed difficulties integrating with CuNW-based TCEs. Those shortcomings are discussed, and how future work might skirt the issues revealed here to produce a very low cost, high performance perovskite solar cell.

Ph.D. / The aim of this study was the development of a new technology for the manufacturing of amorphous silicon (a-Si:H) solar cells on flexible substrates. Kapton R , a commercially available polymer, was used as a substrate to this end. The use of such a polymer, as opposed to glass, results in dramatic savings and also affords the possibility for technological innovation. From the start the project was planned to develop and commission a medium-scale pilot plant manufacturing process. The project thus consisted of two sections: the design, fabrication and implementation of a large-area deposition system, as well as research and development of the materials and cells. A pilot plant was developed and successfully implemented. The optimization of the reactor resulted in very homogeneous materials with good electrical- and optical characteristics. The individual materials were optimized and incorporated into the standard cell configuration (on glass). This process was then transferred to kapton and the configuration was optimized. The use of kapton, as opposed to glass, implies the growth of silicon on a metal film on the kapton. This process leads to a number of phenomena occurring in cells on kapton which do not occur in standard cells on glass. The phenomena include the crystallization of a-Si:H at low temperatures, degradation of the material properties and unwanted microstructure. The origin of these phenomena can be linked to the high occurence of metal/Si-interdiffusion. It was found that this inter-diffusion can be decreased by the insert i on of a thin ZnO buffer layer between the back metal contact and the a-Si:H. The flexible cells were successfully developed and optimized for large areas. An operational manufacturing process was thus developed and the product of this study can now be applied successfully in practical applications.

Two of the main technological challenges of the century are the production of clean energy, on the one hand, and the development of new materials for electronic and spintronic applications that could increase the speed and the storage capacity of regular electronic devices, on the other hand. Organic materials, including fullerenes, organic polymers and organic molecules with metal centres are promising candidates for low-cost, flexible and clean technologies that can address these challenges. A thorough description of the electronic properties of such materials is, therefore, crucial. The interaction of electromagnetic radiation with the molecule can provide the needed insight into the electronic and vibrational levels and on possible chemical interactions. In order to explain and interpret experimentally measured spectra, a good theoretical description of the particular spectroscopy is necessary. Within density functional theory (DFT), the current thesis discusses the theoretical tools used to describe the spectroscopic properties of molecules with emphasis on two classes of organic materials for photovoltaics, molecular electronics and spintronics. Specifically, the stability of the fullerene derivative PC60BM is investigated in connection with its use as an electron acceptor in organic solar cells and the valence band electronic structure of several transition metal phthalocyanines is studied for their possible application in electronics and spintronics. The spectroscopies discussed in the current work are: the photoelectron spectroscopy of the valence band, X-ray photoelectron spectroscopy of the core levels, near-edge X-ray absorption fine structure, Infrared and Raman vibrational spectroscopies

Clean and affordable energy, especially solar energy, is becoming more and more important as our annual total energy consumption keeps rising. However, to make solar energy more affordable and accessible, the cost for fabrication, transportation and assembly of all components need to be reduced. As a crucial component for solar cells, transparent conductive electrode (TCE) can determine the cost and performance. A light weight, easy-to-fabricate and cost-effective new generation TCE is thus needed. While indium-doped tin oxide (ITO) has been the most widely used material for commercial applications as TCEs, its cost has gone up due to the limited global supply of indium. This is not only due to the scarcity of the element itself, but also the massive production of various opto-electronic devices such as TVs, smartphones and tablets. In order to reduce the cost for fabricating large area solar cells, substitute materials for ITO should be developed. These materials should have similar optical transmittance in the visible wavelength range, as well as similar electrical conductivity (sheet resistance) to ITO. This work starts with synthesizing ITO-replacing nano-materials, such as copper nanowires (CuNWs), derivative zinc oxide (ZnO) thin films, reduced graphene oxide (rGO) and so on. Further, we applied various deposition techniques, including spin-coating, spray-coating, Mayer-rod coating, filtration and transferring, to coat transparent substrates with these materials in order to fabricate TCEs. We characterize these materials and analyze their electrical/optical properties as TCEs. Additionally, these fabricated single-material-based TCEs were tested in various lab conditions, and their shortcomings (instability, rigidity, etc.) were highlighted. In order to address these issues, we hybridized the different materials to combine their strengths and compared the properties to single-material based TCEs. The multiple hybridized TCEs have comparable optical/electrical metrics to ITO. The doped-ZnO TCEs exhibit high optical transmittance over 90% in the visible range and low sheet resistance under 200Ω/sq. For CuNW-based composite electrodes, ~ 85% optical transmittance and ~ 25Ω/sq were observed. Meanwhile, the hybridization of materials adds additional features such as flexibility or resistance to corrosion. Finally, as a proof of concept, the CuNW-based composite TCEs were tested in dye-sensitized solar cells (DSSCs), showing similar performance to ITO based samples.