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200944 https://hdl.handle.net/2286/R.2.N.200944 http://rightsstatements.org/vocab/InC/1.0/ All Rights Reserved 2025 150 pages Doctoral Dissertation Academic theses en Amin, Al Yan, Feng FY Yang, Sui SY Li, Lin LL Rolston, Nicholas NR Arizona State University Partial requirement for: Ph.D., Arizona State University, 2025 Field of study: Materials Science and Engineering Antimony selenide (Sb2Se3) has gained significant attention as a promising absorber material for thin-film solar cells due to its excellent anisotropic charge transport and strong light absorption. However, its efficiency remains limited due to challenges in crystal orientation, carrier recombination, and low open-circuit voltage (VOC). This dissertation presents multiple strategies to address these limitations and enhance Sb2Se3 solar cell performance.A key challenge in Sb2Se3 solar cells is the growth orientation of nanoribbons, which affects carrier transport. To promote vertical growth, structural heterostructured CdS buffer layers were employed, facilitating [211] and [221] crystal orientation and improving device efficiency to 7.16%. Similarly, an ultrathin Sb2S3 seed layer was introduced as a template to guide Sb2Se3 nanoribbons along a preferred [002] orientation, achieving an efficiency increase from 5.65% to 7.44%. Additionally, solution-processed Sb2(S,Se)3 seed layers were developed to regulate grain growth, further enhancing the efficiency to 7.52% through improved charge transport and reduced series resistance. To tackle VOC limitations, inorganic vanadium oxide (VOx) was incorporated as a hole transport layer (HTL). The VOx layer significantly enhanced the built-in potential (Vbi), leading to an increase in device efficiency from 5.5% to 6.3%. Another major challenge, selenium deficiency in Sb2Se3 films, was addressed through a rapid thermal selenization (RTS) technique. RTS effectively replenished selenium vacancy defects while preventing unwanted interdiffusion CdS window and Sb2Se3 absorber layer, achieving a record efficiency of 8.25%. Overall, these advancements in interface engineering, grain orientation control, and material modifications provide a comprehensive strategy for realizing high-efficiency Sb₂Se₃ thin-film solar cells. The methodologies presented in this dissertation pave the way for further development of antimony chalcogenide photovoltaics, bringing them closer to their theoretical efficiency limit. Materials Science Interfacial Engineering of Antimony Selenide Thin Film Solar Cells