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研究生： 周啟達
Chi-Ta Chou
論文名稱： 有機分子堆疊排列致高開路電壓有機太陽能電池
Stacking orientation mediation of pentacene and derivatives for high open-circuit voltage organic solar cells
指導教授： 戴龑
Yian Tai
口試委員: 劉進興
Chin-Hsin J. Liu
陳貴賢
Kuei-Hsien Chen
林麗瓊
Li-Chyong Chen
黃智賢
Jih Shang Hwan
學位類別： 博士
Doctor
系所名稱： 工程學院 - 化學工程系
Department of Chemical Engineering
論文出版年： 2012
畢業學年度： 100
語文別： 英文
論文頁數： 153
中文關鍵詞： 有機太陽能電池 、開路電壓 、分子排列
外文關鍵詞： VOC
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    • 有機太陽能電池中，有機分子的排列堆疊的方式是影響太陽能電池效率的其中一個重要關鍵。本研究利用五聯苯 (pentacene)及其衍生物探討高開路電壓有機太陽能電池。此研究中，分別利用兩個不同的五聯苯衍生物，均在五聯苯的主幹上加上苯環基團，為6,13-dipheynl-pentacene (DP-Penta)及 6,13-Di-bipheynl-4- yl-pentacene (DB-Penta)。利用變角度的X光吸收近邊緣結構(near-edge X-ray absorption fine structure, NEXAFS)量測可得知五聯苯及其衍生物成膜後於基板上具有不同的分子排列，五聯苯為依著長軸站立於PEDOT:PSS表面上，而具有與聯苯主幹垂直之苯環基團的兩個五聯苯衍生物則是平躺於基板表面上。由此材料製做成的小分子有機太陽能電池有很大的差異，利用DB-penta/C60所製作的元件，相對於pentacene/C60的參考標準元件，其開路電壓(Voc)由0.28V提高至0.83V，有明顯的提升。這是因為分子排列平躺著的五聯苯衍生物能夠與上層的C60具有較好的π-π overlap，使得在p-n界面中具有新的電荷分佈，促使真空能階的偏移，更進一步的影響並增加元件的開路電壓。此研究結果可以延伸引用到其他的有機太陽能電池系統，可以有效的增加影響其元件效率。

    Molecular stacking orientation is one of the major factors for high performance in organic solar cells. Here, we study the open-circuit-voltage (VOC) of organic heterojunction photovoltaic cells based on pentacene and its derivatives. Two functionalized forms of pentacene- 6,13-dipheynl-pentacene (DP-Penta) and 6,13-Di-bipheynl-4-yl-pentacene (DB-Penta)– have been used for this study. Different molecular stacking orientations of the pentacene-derivatives have been identified by angle dependent near-edge X-ray absorption fine structure (NEXAFS) measurements. It’s concluded that pentacene molecules stand up on the PEDOT:PSS surface, while functionalized pentacene molecules lie down on the surface upon the modification of additional orthogonal phenyl rings. A significant increase of the VOC from 0.28 to 0.83 V has been observed when a conventional pentacene/C60 cell is replaced by the DB-penta/C60 cell. This result can be attributed to the fact that down-lying molecular stacking orientation of the functionalized pentacene induced a vacuum level (V. L.) shift, resulting in improved VOC of the devices. This approach has important implications for organic electronic devices that comprise multiple organic layers, and particularly for improving the power conversion efficiency of organic photovoltaic cells.

    Chapter 1 Introduction 11 1.1 Photovoltaic Technology Overview 13 1.2 Why Organic Photovoltaic? 16 1.3 OPV Device Architectures 18 1.3.1 Planar Bilayer 18 1.3.2 Bulk Heterojunctions 20 1.3.3 Interfacial Layers 21 1.4 The Importance of Molecular Orientation Effect in OPV 26 1.5 Photovoltaic Device Characterization 29 1.5.1 Efficiency Measurements 29 1.5.2. Equivalent Circuit Model 34 Chapter 2 Knowledge of OPV 36 2.1 Basic Properties of Organic Semiconductors 36 2.1.1 Materials and the Chemical Properties 36 2.1.2 Optical Properties 42 2.1.3 Electric Properties 46 2.1.4 Exciton Diffusion Length, LD 49 2.2 Component Materials of OPV Devices 50 2.2.1 Substrate 50 2.2.2 Transparent Electrode 52 2.2.3 Active Layer 54 2.2.3.1. Phthalocyanines 56 2.2.3.2. Polyacenes 62 2.2.3.3. Other Electron-Donating Materials 63 2.2.3.4. Fullerenes 67 2.2.4. Back Electrode 71 2.3 Interfacial Electronic Structures and Energy Level Alignment 73 2.3.1 Organic Solid Electronic Structure 74 2.3.2 Vacuum Level Definition 77 2.3.3 Interfacial Energy Level Alignment 80 2.3.4 The Factors of Interfacial Dipole Layer 82 Chapter 3 Experimental 86 3.1 Organic Thin Film Deposition 86 3.2 Thin Film Characterization 88 3.2.1 Optical Absorption Spectroscopy 88 3.2.2 Ultraviolet Photoemission Spectroscopy (UPS) 89 3.2.3 Angle-dependent Near Edge X-ray Absorption Fine Structure (NEXAFS) 91 3.3 Device Characterization 91 3.3.1 Device Fabrication 91 3.3.2 Current-Voltage (IV ) Measurement 93 3.3.3 Incident Photon-to-Electron Conversion Efficiency (IPCE) Measurement 93 Chapter 4 Result and Discussion 96 4.1 Basic Introduction and Pentacene Derivatives 96 4.2 Thickness Dependent of Pentacene-Derivatives OPV Devices 99 4.3 Comparison with Reference Cell 109 4.4 Energy Level Alignment of OPV 112 4.5 Molecular Orientation of Donor Materials 119 4.6 C70 for Acceptor Material 124 Chapter 5 Conclusion 130 Reference 131 Appendix-1 149 Appendix-2 151

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