This dissertation, "Organic Solar Cells Towards High Efficiency: Plasmonic Effects and Interface Engineering" by Chuandao, Charlie, Wang, 王传道, was obtained from The University of Hong Kong (Pokfulam, Hong Kong) and is being sold pursuant to Creative Commons: Attribution 3.0 Hong Kong License. The content of this dissertation has not been altered in any way. We have altered the formatting in order to facilitate the ease of printing and reading of the dissertation. All rights not granted by the above license are retained by the author. Abstract: Organic solar cells (OSCs) are promising candidates for solar light harvesting due to their standout advantages both in material properties and manufacturing process. During past decades, remarkable progress has been achieved. Efficiency for single-junction cells over 9% and tandem cells over 10% has been reported. For high performance OSCs towards commercialization, sufficient light absorption and high quality buffer layers are still two challenges, which are addressed in this thesis by investigating the plasmonic effects on OSCs and interface engineering. Here, the mechanisms of plasmonic effects on OSC are explored by incorporating metallic Au nanoparticles (NPs) in individual anode buffer layer and active layer, respectively, and finally in both layers simultaneously. When Au NPs are incorporated into the buffer layer, surface plasmonic resonance (SPR) induced absorption enhancement due to incorporation of Au NPs is evidenced theoretically and experimentally to be only minor contributor to the performance improvement. The increased interfacial contact area between the buffer layer and active layer, together with the reduced resistance of the buffer layer due to the embedded Au NPs, are revealed to benefit hole collection and thus are main contributors to the performance improvement. When Au NPs are embedded in the active layer, Au NPs induced SPR indeed contributes to enhanced light absorption. However, when large amount of Au NPs are incorporated, the negative effects of NPs on the electrical properties of OSCs can counter-diminish the optical enhancement from SPR, which limits the overall performance improvement. When Au NPs are embedded into both layers, both advantages of incorporating NPs in individual layers can be utilized together to achieve more pronounced improvement in photovoltaic performance; as a result, accumulated enhancements in device performance can be achieved. The results herein are applicable to other metallic NPs such as Ag NPs, Pt NPs, etc. The study herein has clarified the degree of contribution of SPR effects on OSCs and revealed the mechanisms behind. It has also highlighted the importance of considering both optical and electrical effects when employing metallic NPs as strategies to enhance the photovoltaic performance of OSCs. Consequently, the study contributes both physical understanding and technological development of applying metallic NPs on OSCs. Regarding interface engineering, we first propose a simple method to modify the substrate work function for efficient hole collection by using an ultra-thin ultraviolet-ozone treated Au. The method can be used in other situations such as modifying the work function of multilayer graphene as transparent electrode. Then we propose a general method to synthesize solution-processed transition metal oxides (TMOs). Besides high material quality, desirable electrical properties, and good stability, our method stands out particular in that the synthesized TMOs can be dispersed in water-free solvents and the TMO films require only low temperature treatment, which is very compatible with the organic electronics. Our method can also be used to synthesize other TMOs other than the demonstrated molybdenum oxide and vanadium oxide. The proposed method herein is applicable in semiconductor industry. DOI: 10.5353/th_b4832965 Subjects: Solar cells