In polycrystalline thin-film cadmium telluride (CdTe) solar cells, atomic defects (dopants: copper (Cu), arsenic (As); and selenium (Se) alloy) have significantly enhanced hole density and minority carrier lifetime. Density functional theory (DFT) has predicted the atomic configurations of relevant defects and their electronic structures. Yet, experimental evidence of the defects, especially their spatial distribution across the absorber, is still lacking. Herein, since it can probe local atomic structure of elements of interest with trace-elemental sensitivity, nanoprobe X-ray absorption near edge structure (XANES) spectroscopy was used to elucidate atomic structures of Cu, As, and Se. After XANES spectra were measured from CdTe devices, the atomic information was extracted from the measured spectra by fitting them with reference spectra, which were simulated from 1) point defects and grain boundaries (GBs) predicted by DFT; 2) secondary phases which could form under processing conditions. XANES analysis of various device architectures revealed structural inhomogeneities across the absorbers from point defects to secondary phases. The majority of the Cu dopant atoms form secondary phases with surrounding atoms even inside the absorbers, explaining the low dopant activation. When entering the target lattice site (Cd), Cu forms a complex with chlorine (Cl) and becomes a donor defect, compensating hole density. Compared to Cu, As dopant tends to enter the target site (Te) more frequently, explaining higher hole density in As-doped CdTe. Notably, As on the Te site forms neutral charged complexes with Cl. Although they are not as detrimental as the Cu-Cl complex, the As-Cl complexes may be responsible for low dopant activation and compensation observed in As-doped CdTe devices. Complementary to the DFT prediction, this work provided the distribution of Se local structures across the absorber, specifically the variation of Se-Cd bond lengths in differently performing areas. Under environmental stressors (heat and light), it showed atomic reconfiguration of Se and Cl at GBs, and Se diffusion into the bulk, co-occurring with device degradation. This framework was also extended to study defect evolution in other thin-film solar cells (CIGS and emerging perovskite). XANES analysis has shed light on atomic defects governing solar cell performance and stability, which are crucial in pushing the efficiency toward the theoretical efficiency limit.

Layered oxyhalide magnetic materials have recently emerged as one of the most promising material systems in the field of spintronics and quantum devices because of their large optical anisotropy, magnetic phase transition associated with structural changes, strong antiferromagnetism coupled with weak interlayer bonding and high environmental stability. Despite their attractive magnetic properties and outstanding environmental stability, bottom-up approaches for scalable growth remain limited due to presence of coexisting phases with different stoichiometry in their phase diagram.This work presents the first synthesis of environmentally stable ultra-thin flakes of oxyhalide magnetic CrOCl on Mica and Sapphire substrates using CrCl¬3 and KMnO4 as precursor materials through Atmospheric-Pressure Chemical Vapor Deposition (APCVD) technique in the presence of Argon carrier gas. Comprehensive characterization techniques such as Scanning Electron Microscopy (SEM), Energy Dispersive Spectroscopy (EDS) and X-ray Diffraction (XRD) were employed to confirm the stoichiometry and crystallinity of the grown CrOCl flakes. The findings of the work revealed that the quality of the CrOCl flakes depends on the concentration of the oxygen radicals provided by KMnO4 precursor and substrate temperature. Moreover, morphology and the phase of the material are strongly affected by a variety of factors such as the carrier gas flow rate, the growth time, and the growth temperature. Overall, this work expands the fundamental understanding of the bottom-up growth mechanisms involved in synthesizing such materials thereby contributing to the expansion of the library of stable magnetic oxides with potential applications in advanced technological devices.

The silicon-based solar cell has been extensively deployed in photovoltaic industry and plays an important role in renewable energy industries. A more energy-efficient, environment-harmless and eco-friendly silicon production technique is required for price-competitive solar energy harvesting. Silicon electrorefining in molten salt is promising for the ultrapure solar-grade Si production. To avoid using highly corrosive fluoride salt, CaCl2-based salt is widely employed for silicon electroreduction. For Si electroreduction in CaCl2-based salt, CaO is usually added to enhance the solubility of SiO2. However, the existence of oxygen in molten salt could result in system corrosion, anode passivation and the co-deposition of secondary phases such as CaSiO3 and SiO2 at the cathode. This research focuses on the development of reusable oxygen-free CaCl2-based molten salt for solar-grade silicon electrorefining. A new multi-potential electropurification process has been proposed and proven to be more effective in impurities removal. The as-received salt and the salt after electrorefining have been electropurified. The inductively-coupled plasma mass spectrometry and cyclic voltammetry have been utilized to determine the impurities removal of electropurification. The salt after silicon electrorefining has been regenerated to its original purity level before by the multi-potential electropurification process, demonstrating the feasibility of a reusable salt by electropurification. In an oxygen-free CaCl2-based salt without silicon precursor, the silicon dissolved from the silicon anode can be successfully deposited at the cathode. The silicon anode has been operated for more than 50 hours without passivation in the oxygen-free system. Silicon ions start to be deposited after 0.17 g of silicon has been dissolved into the salt from the silicon anode. A 180 µm deposit with a silver-luster surface was obtained at the cathode. The main impurities in the silicon anode such as aluminum, iron and titanium were not found in the silicon deposits. No oxygen-containing secondary phases are detected in the silicon deposits. These results confirm the feasibility of silicon electrorefining in the oxygen-free CaCl2-based salt.

Applications like integrated circuits, microelectromechanical devices, antennas, sensors, actuators, and metamaterials benefit from heterogeneous material systems made of metallic structures and polymer matrixes. Due to their distinctive shells made of metal and polymer, scaly-foot snails, which are found in the deep ocean, exhibit high strength and temperature resistance. Recent metal deposition fabrication techniques have been used to create a variety of multi-material structures. However, using these complex hybrid processes, it is difficult to build complex 3D structures of heterogeneous material with improved properties, high resolution, and time efficiency. The use of electrical field-assisted heterogeneous material printing (EFA-HMP) technology has shown potential in fabricating metal-composite materials with improved mechanical properties and controlled microstructures. The technology is an advanced form of 3D printing that allows for printing multiple materials with different properties in a single print. This allows for the creation of complex and functional structures that are not possible with traditional 3D printing methods. The development of a photocurable printing solution was carried out that can serve as an electrolyte for charge transfer and further research into the printing solution's curing properties was conducted. A fundamental understanding of the formation mechanism of metallic structures on the polymer matrix was investigated through physics-based multiscale modeling and simulations. The relationship between the metallic structure's morphology, the printing solution's properties, and the printing process parameters was discovered.The thesis aims to investigate the microstructures and electrical properties of metal-composite materials fabricated using EFA-HMP technology and to evaluate the correlation between them. Several samples of metal-composite materials with different microstructures will be fabricated using EFA-HMP technology to accomplish this. The results of this study will provide a better understanding of the relationship between the microstructures and properties of metal-composite materials fabricated using EFA-HMP technology and contribute to the development of new and improved materials in various fields of application. Furthermore, this research will also shed light on the advantages and limitations of EFA-HMP technology in fabricating metal-composite materials and study the correlation between the microstructures and mechanical properties.