本研究主要是以溶膠凝膠法製備氧化鋅薄膜，作為內部光萃取結構應用於有機發光二極體，使其有效降低元件內部的光損耗，提升元件的光萃取效率及外部量子效率(EQE)，並成功應用在可撓式有機發光二極體。
首先我們將氧化鋅溶膠凝膠進行不同體積莫耳濃度配製，探討其成膜後之差異，並對其做穿透度、光學特性、表面形態之量測與探討，接著進行ITO陽極圖型化之設計與製作。
我們首先進行藍光OLED元件的優化，然後應用在具氧化鋅薄膜的微結構基板上，並製作出具有內部光萃取結構之藍光OLED元件，後續進行元件的光電特性量測，探討光萃取結構對藍光OLED元件的光電特性影響。
最後本實驗成功的利用濃度為0.6 M所製作的氧化鋅薄膜製作出具有內部光萃取結構的藍光OLED元件，其外部量子效率在亮度為1000cd/m2時的增進約20%。並藉由提高烘烤溫度，大幅增加光萃取元件之再現性及穩定性，並且成功製作在PEN軟性基板上。

In this study, we fabricated organic light-emitting diodes (OLEDs) with internal light extraction structure to reduce the Waveguide mode loss and increase the EQE by using the Sol–gel-deposited ZnO light extraction thin films. And successfully fabricated the organic light-emitting diodes on flexible plastic substrate.
First, we prepare different ratio of the zinc oxide (ZnO) sol-gel to form various thickness of ZnO thin films by using different spin rate. We investigated surface morphology and optical characteristics of the ZnO thin films, and then, design and fabrication of ITO anodes were performed.
The optimized standard blue OLED device structures were chosen to fabricate blue OLEDs with internal light extraction structure. The opto-electrical properties of the devices were measured and studied.
Finally, we successfully fabricated blue OLEDs with the Sol–gel-deposited ZnO light extraction thin films. Significantly, the blue OLEDs with internal light extraction structure have great light extraction efficiency which increase the external quantum efficiency (EQE) by 20% compared to standard OLEDs at 1000cd/m2. We can inprove the reality and stability of OLED with ZnO light extraction thin films by increasing the baking temperature. And successfully fabricated the organic light-emitting diodes on flexible plastic substrate.

中文審定書 i
英文審定書 ii
致謝 iii
中文摘要 iv
Abstract v
目錄 vii
圖目錄 x
表目錄 xiii
第一章 緒論 1
1-1 前言 1
1-2 有機發光二極體的歷史進展 1
1-3 OLED元件的結構介紹 3
1-3-1 雙層A型 3
1-3-2 雙層B型 4
1-3-3 三層A型 4
1-3-4 三層B型 5
1-4 OLED元件的基本發光原理 6
1-4-1 有機與無機發光機制比較 6
1-4-2 有機發光二極體基礎理論 8
1-4-3 能量轉換機制 10
1-5 有機電激發光元件材料介紹 12
1-5-1 陽極 13
1-5-2 電洞注入層 13
1-5-3 電洞傳輸層 14
1-5-4 高分子發光層 14
1-5-5 小分子發光層 15
1-5-6 電子傳輸層 15
1-5-7 電子注入層 16
1-5-8 陰極 16
1-6 摻雜技術 16
1-7 濃度淬息效應 18
1-8 三重態自我毀滅現象 19
1-9 發光效率定義 19
1-10 光色鑑定 21
1-11 OLED光學損耗因素 22
1-12 研究動機 23
1-13 文獻回顧 24
第二章 實驗方法與流程 26
2-1 實驗架構 26
2-2 實驗材料 27
2-3 實驗設備 29
2-3-1 製程設備 29
2-3-2 量測設備 32
2-4 有機發光二極體實驗步驟 36
2-4-1 基板清潔 36
2-4-2 溶膠凝膠氧化鋅配製及成膜 36
2-4-3 濺鍍圖案化ITO(Sputter-pattenred ITO)製程 37
2-4-4 有機薄膜與金屬薄膜蒸鍍製程 38
2-4-5 OLED元件之封裝製程 40
2-4-6 OLED元件之量測 41
第三章 結果與討論 42
3-1 配製0.4 M之氧化鋅薄膜 42
3-1-1 薄膜穿透率分析 42
3-1-2 薄膜光學特性分析 43
3-1-3 薄膜表面形態分析 44
3-1-4 製程元件數據分析 45
3-1-5 結論 47
3-2 配製0.6 M之氧化鋅薄膜 47
3-2-1 薄膜表面形態分析 47
3-2-2 製程元件數據分析 48
3-2-3 結論 50
3-3 提升0.6 M烤乾溫度之氧化鋅薄膜 50
3-3-1 薄膜穿透率分析 50
3-3-2 薄膜表面形態分析 51
3-3-3 製程元件數據分析 52
3-3-4 結論 54
3-4 配製0.8 M之氧化鋅薄膜 54
3-4-1 薄膜穿透率分析 54
3-4-2 薄膜表面形態分析 55
3-4-3 製程元件數據分析 56
3-4-4 結論 58
3-5 軟性基板元件製程 58
第四章 總結 61
參考文獻 62

[1] Pope, M., Kallmann, H. P., & Magnante, P. (1963). Electroluminescence in organic crystals. The Journal of Chemical Physics, 38(8), 2042-2043.
[2] Tang, C. W., & VanSlyke, S. A. (1987). Organic electroluminescent diodes. Applied physics letters, 51(12), 913-915.
[3] Burroughes, J. H., Bradley, D. D. C., Brown, A. R., Marks, R. N., Mackay, K., Friend, R. H., ... & Holmes, A. B. (1990). Light-emitting diodes based on conjugated polymers. Nature, 347(6293), 539-541.
[4] Lee, J. Y., Connor, S. T., Cui, Y., & Peumans, P. (2008). Solution-processed metal nanowire mesh transparent electrodes. Nano letters, 8(2), 689-692.
[5] Adachi, C., Tokito, S., Tsutsui, T., & Saito, S. (1988). Organic electroluminescent device with a three-layer structure. Japanese journal of applied physics, 27(4A), L713.
[6] Era, M., Adachi, C., Tsutsui, T., & Saito, S. (1991). Double-heterostructure electroluminescent device with cyanine-dye bimolecular layer as an emitter. Chemical physics letters, 178(5-6), 488-490.
[7] Kido, J., Kohda, M., Okuyama, K., & Nagai, K. (1992). Organic electroluminescent devices based on molecularly doped polymers. Applied physics letters, 61(7), 761-763.
[8] Kido, J., Kimura, M., & Nagai, K. (1995). Multilayer white light-emitting organic electroluminescent device. Science-new york then washington-, 1332-1332.
[9] Kido, J., Shionoya, H., & Nagai, K. (1995). Single‐layer white light‐emitting organic electroluminescent devices based on dye‐dispersed poly (N‐vinylcarbazole). Applied physics letters, 67(16), 2281-2283.
[10] Kafafi, Z. H. (Ed.). (2005). Organic electroluminescence. Crc press.
[11] Sze, S. M. (2008). Semiconductor devices: physics and technology. John Wiley & Sons.
[12] Miyata, S. (1997). Organic electroluminescent materials and devices. Crc press.
[13] Sugiyama, K., Yoshimura, D., Miyamae, T., Miyazaki, T., Ishii, H., Ouchi, Y., & Seki, K. (1998). Electronic structures of organic molecular materials for organic electroluminescent devices studied by ultraviolet photoemission spectroscopy. Journal of applied physics, 83(9), 4928-4938.
[14] Chen, X. W., Choy, W. C., Liang, C. J., Wai, P. K. A., & He, S. (2007). Modifications of the exciton lifetime and internal quantum efficiency for organic light-emitting devices with a weak/strong microcavity. Applied physics letters, 91(22), 221112.
[15] Tang, C. W., VanSlyke, S. A., & Chen, C. H. (1989). Electroluminescence of doped organic thin films. Journal of applied physics, 65(9), 3610-3616.
[16] 陳金鑫, & 黃孝文. (2005). OLED: 有機電激發光材料與元件. 五南圖書出版股份有限公司.
[17] Förster, T. (1948). Zwischenmolekulare energiewanderung und fluoreszenz. Annalen der physik, 437(1‐2), 55-75.
[18] Dexter, D. L. (1953). A theory of sensitized luminescence in solids. The journal of chemical physics, 21(5), 836-850.
[19] Miyata, S. (1997). Organic electroluminescent materials and devices. Crc press.
[20] Van Slyke, S. A., Chen, C. H., & Tang, C. W. (1996). Organic electroluminescent devices with improved stability. Applied physics letters, 69(15), 2160-2162.
[21] Mashford, B. S., Stevenson, M., Popovic, Z., Hamilton, C., Zhou, Z., Breen, C., ... & Kazlas, P. T. (2013). High-efficiency quantum-dot light-emitting devices with enhanced charge injection. Nature photonics, 7(5), 407-412.
[22] Sasabe, H., Nakanishi, H., Watanabe, Y., Yano, S., Hirasawa, M., Pu, Y. J., & Kido, J. (2013). Extremely Low Operating Voltage Green Phosphorescent Organic Light‐Emitting Devices. Advanced functional materials, 23(44), 5550-5555.
[23] Jeon, W. S., Park, J. S., Li, L., Lim, D. C., Son, Y. H., Suh, M. C., & Kwon, J. H. (2012). High current conduction with high mobility by non-radiative charge recombination interfaces in organic semiconductor devices. Organic electronics, 13(6), 939-944.
[24] Cho, S. H., Pyo, S. W., & Suh, M. C. (2012). Low voltage top-emitting organic light emitting devices by using 1, 4, 5, 8, 9, 11-hexaazatriphenylene-hexacarbonitrile. Synthetic metals, 162(3), 402-405.
[25] Van Slyke, S. A., Chen, C. H., & Tang, C. W. (1996). Organic electroluminescent devices with improved stability. Applied physics letters, 69(15), 2160-2162.
[26] Stolka, M., Yanus, J. F., & Pai, D. M. (1984). Hole transport in solid solutions of a diamine in polycarbonate. The journal of physical chemistry, 88(20), 4707-4714.
[27] Shoustikov, A. A., You, Y., & Thompson, M. E. (1998). Electroluminescence color tuning by dye doping in organic light-emitting diodes. IEEE journal of selected topics in quantum electronics, 4(1), 3-13.
[28] Baldo, M. A., Adachi, C., & Forrest, S. R. (2000). Transient analysis of organic electrophosphorescence. II. Transient analysis of triplet-triplet annihilation. Physical review b, 62(16), 10967.
[29] Sun, Y., & Forrest, S. R. (2007). High-efficiency white organic light emitting devices with three separate phosphorescent emission layers. Applied physics letters, 91(26), 263503.
[30] 顧鴻壽. (2001). 光電有機電激發光顯示器技術及應用. 新文京開發.
[31] Bocksrocker, T., Preinfalk, J. B., Asche-Tauscher, J., Pargner, A., Eschenbaum, C., Maier-Flaig, F., & Lemme, U. (2012). White organic lightemitting diodes with enhanced internal and external outcoupling for ultra-efficient light extraction and Lambertian emission. Optics express, 20(106), A932-A940..
[32] Galeotti, F., Mróz, W., Scavia, G., & Botta, C. (2013). Microlens arrays for light extraction enhancement in organic light-emitting diodes: a facile approach. Organic electronics, 14(1), 212-218.
[33] Kim, D. H., Kim, J. Y., Kim, D. Y., Han, J. H., & Choi, K. C. (2014). Solution-based nanostructure to reduce waveguide and surface plasmon losses in organic light-emitting diodes. Organic electronics, 15(11), 3183-3190.
[34] Chen, C. Y., Lee, W. K., Chen, Y. J., Lu, C. Y., Lin, H. Y., & Wu, C. C. (2015). Enhancing Optical Out‐Coupling of Organic Light‐Emitting Devices with Nanostructured Composite Electrodes Consisting of Indium Tin Oxide Nanomesh and Conducting Polymer. Advanced materials, 27(33), 4883-4888.
[35] Kim, K. H., & Park, S. Y. (2016). Enhancing light-extraction efficiency of OLEDs with high-and low-refractive-index organic–inorganic hybrid materials. Organic electronics, 36, 103-112.
[36] 黃智國. (2016) “可撓曲式電極與光萃取結構應用於有機電激發光二極體之研究” 中山大學博士論文.
[37] 陳一帆. (2005) “RF濺鍍式ITO薄膜沉積之後熱處裡效應 ” 中山大學碩士論文.
[38] 洪培元. (2016) “以內部光萃取結構增進有機電激發光二極體效率之研究” 中山大學碩士論文.