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(2023)ThesisDue to the unique photovoltaic properties and ease of fabrication, organic-inorganic halide perovskites have generated considerable research interest. The perovskite solar cell can be applied to many applications, by tuning the bandgap. Inter of Things (IoT) devices and tandem solar cell applications, in particular, have been required for the wide bandgap perovskite solar cells. However, wide bandgap perovskite solar cells have band alignment mismatch problems, leading to charge recombination at the interface of perovskite, resulting in encouraging low device performance and decrease device stability. The first part of this thesis includes the study of the structure and working mechanism of perovskite solar cells. In addition, the defect of the perovskite was explained about how the majority of defects formed. This is caused by shallow defect energies within the bandgap, low density of deep traps, and low trap-charge interaction cross-sections which are occurred during the interaction between traps and charges. After that, the explanation of the reason how wide bandgap is applied for the indoor application. There is previous work on the tuning of the band alignment between perovskite and hole transfer layer which improved the efficiency of hole transfer, resulting in high device performance under the low light intensity condition. Lastly, the experiment of the thesis is focused on the address of the band alignment mismatch by adding two dimensional (2D) BA2PbBr4 perovskite layer for the tunnelling effect between the electron transport layer (ETL) and perovskite layer. The tunnelling layer of 2D perovskite improved the 3D perovskite crystal quality and charge transport from the 3D perovskite to ETL. As a result, the power conversion efficiency under the 200 lux white light emitting diodes (LED) light for the IoT devices was 43.70% with around 1 V of open circuit voltage and improved the device stability under the 1000 lux of white LED up to 1200 hrs.
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(2018)ThesisGraphene oxide is a single layer of carbon atoms with decorated oxygen functional groups. Stacked monolayers in the laminate form create an interlayer space of sub-nanometer scale with oxygenated functional group to attract water molecules, and graphitic domains to allow frictionless flow of water molecules and achieve maximum efficiency of water transportation. The research reported herein is aimed to understand and explore characteristics of the diffusion-dependent mass transportation across an array of cascading nanochannels confined by graphene oxide laminates at sub-nanometer level. This dissertation has 6 Chapters. Chapter 1 is the introduction and Chapter 2 reports the recent progress in graphene oxide for mass transport application. Chapter 3 discusses efforts of engineering the channel confinement, which is represented by the interlayer spacing in between graphene oxide laminates. By adjusting the fundamental factors of graphene oxide suspension, the interlayer spacing can be controlled at 0.7 to 0.8 nm. Based on the engineered interlayer spacing, separation of vaporous mixture by graphene oxide membrane is studied in Chapter 4. Numerical description of nanochannels enclosed by graphene oxide monolayers is determined by time lag analysis. The feature of ethanol vapor transportation with the support of water vapor is revealed, showing accelerated transportation of non-permeable matter, which enriches the existing knowledge. A geometrical model of graphene oxide membrane for vapor separation was established and analyzed. In Chapter 5, adsorption and intercalated of molecules and solvated ions are studied and proved as a size-dependent enlargement of graphene oxide nanochannels. Carriers such as water and ethanol are used for transporting ions and molecules into graphene oxide slits. Taking the adsorption into consideration, permeation of vaporous substances through adsorbed graphene oxide membrane is investigated in Chapter 6. The research initiates researching crystallization of adsorbed matters in graphene oxide interlayer structure. A simplified model was directed to predict the water vapor permeation behavior of intercalated graphene oxide membrane. Such efforts not only lead to a better understating of graphene oxide membrane for gas separation but also give a hint of spatially efficient matter transport in achieving excellent electrochemical devices with graphene oxide components.
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(2022)ThesisMultijunction solar cells based on silicon are predicted to achieve an efficiency of 40-45% for a top cell with a band gap of 1.6-1.9 eV. However, there are currently no known materials with suitable band gaps able to deliver high efficiencies. Two classes of materials that have been proposed for top cells are alloys of CuGaSe2 and alloyed oxide perovskites. CuGaSe2 has a suitable band gap (1.68 eV) for a top cell on silicon, but the maximum efficiency achieved is only 11%, while that of the closely-related CuInGaSe2 (band gap 1.14 eV) is 23.35%. The low efficiency of CuGaSe2 has been attributed to anti-site defects. Therefore, suppressing this defect formation is critical to achieving higher efficiencies. On the other hand, most oxide perovskites have band gaps that are too high (>2 eV) to be used as top cells on silicon, hence strategies such as alloying are required to lower their band gaps. In this work, the effects of alloying CuGaSe2 with Ag, Na, K, Al, In, La and S were investigated using Density Functional Theory (DFT) calculations. The band gaps of the alloyed compounds and formation energies of anti-site defects were calculated to find alloying elements that can increase the defect formation energy but maintain the band gap. CuGaSe2 alloyed with Al at 50at% showed the highest increase (compared to unalloyed CuGaSe2) in the defect formation energy (by ~0.20 eV) followed by Na (~0.15 eV) and S (~0.10 eV), both at 50at%. However, the band gap of the Al alloy (~2.15 eV) is too high for a top cell, while those of Na (~1.95 eV) and S (~1.91 eV) are slightly above the upper limit. Thus, alloying with these elements is not an ideal route towards significantly increasing the formation energy of anti-site defects while maintaining the band gap of CuGaSe2. However, some of the factors that influence the defect formation energy are identified, potentially leading to design rules for future work. Defect formation energies were found to be higher in structures with more positively charged Ga and negatively charged Se atoms. Analysis of bond lengths revealed a positive correlation between shorter Ga and Se bonds and higher defect formation energies. Band gaps of various alloyed oxide perovskites were calculated using DFT. BiFeO3 was alloyed with Y and Sb; LaFeO3 with Cr and Sb and YFeO3 with Bi and Sb. YFeO3 alloyed with Sb at 50at%, was found to have a band gap of 1.4-2.1 eV (depending on the basis set used) which is in the range for a top cell.