本研究是利用商售之二氧化鋯、熱固型矽樹脂以及丙二醇甲醚醋酸酯(propylene glycol methyl ether acetate, PGMEA)混合成散射膜溶液後，以旋轉塗佈法將溶液塗佈於玻璃基板上，熱處理後形成散射膜。
在本文中散射膜溶液的製備方法主要分為兩種，第一種方式是將散射膜溶液以機械均質法的方式進行分散，再將溶液以磁石攪拌混合均勻後，進行散射膜的塗佈；第二種是以球磨法來進行分散，改變球磨時的ZrO2濃度、鋯珠直徑、球磨時間等製程參數，製備出具有不同表面粗糙度的散射膜，並藉由控制散射膜的厚度，對散射膜溶液進行三段球磨等步驟，以製造具有更低表面粗糙度的散射膜，在實驗的最後我們成功製備出Pa與Pz值分別為48.8與298奈米的平坦散射膜。
我們除了探討不同製程參數對散射膜表面性質的影響之外，我們也會針對不同製程參數所製備的散射膜所表現的光學性質進行討論，並將製造出來的散射膜應用於有機發光二極體(organic light-emitting diode, OLED)上，觀察其對OLED效率和光學性質的影響；從散射膜應用於OLED的效果，我們發現所有包含ZrO2的散射膜都可以促進OLED的效率並降低其隨視角變化的色座標變化值。

In this study, composite scattering films were formed by spin coating the mixing solution on glass substrates. The mixing solution was composed of commercial zirconia nano-powders, thermosetting silicone resin, and propylene glycol methyl ether acetate.
In this article, the preparation methods of the mixing solution were mainly divided into two types. In the first method, zirconia nano-powders were dispersed in the mixing solution by a mechanical homogenizer and a magnetic stir. In the second method, zirconia nano-powders were dispersed in the mixing solution by a ball miller. Composite scattering films, having various surface roughness, were fabricated by varying the zirconia concentration in the mixing solution, diameters of zirconia beads, treating time, and other process parameters during the ball milling. In order to possess a lower surface roughness of composite scattering films, a tertiary ball-milling treatment was introduced to disperse zirconia nano-powders in the mixing solution. At the end of the experiment, we successfully prepared a flat scattering film with Pa and Pz values of 48.8 and 298 nm, respectively.
In addition to study the influences of different process parameters on the surface morphology and optical properties of composite scattering films, we will also apply composite scattering films to an organic light-emitting diode to investigate its efficiency and optical properties; from the effect of scattering film applied to OLED, we found that all scattering films containing ZrO2 can promote the efficiency of OLED and reduce its max CIE change value with viewing angle.

第 一 章 序論 1
1.1 前言 1
1.2 研究動機 2
1.3 文獻回顧 2
1.3.1 有機發光二極體(OLED)與波導效應 2
1.3.2 OLED光萃取結構 5
1.3.3 散射膜製備方式與其應用 7
1.3.4 粉體分散技術 10
第 二 章 理論基礎 15
2.1 司乃耳定律 15
2.2 光散射 16
2.3 機械均質分散 17
2.4 球磨分散[23] 17
2.5 表面粗糙度[24-26] 17
2.6 霧度與穿透度 20
2.7 OLED效率增益 22
2.8 CIE色彩色座標系統 23
第 三 章 實驗步驟與量測方式 25
3.1 散射膜製程 25
3.1.1 機械均質 26
3.1.2 球磨 27
3.1.3 溶液塗佈 28
3.2 性質分析 29
3.2.1 表面形貌分析 29
3.2.2 霧度與穿透度量測 30
3.2.3 輝度與色座標量測 30
3.3 設備與儀器 30
3.3.1 機械均質機 31
3.3.2 球磨機 32
3.3.3 高功率細胞破碎機 32
3.3.4 超音波清洗機 33
3.3.5 加熱板 33
3.3.6 旋轉塗佈機 34
3.3.7 掃描式電子顯微鏡 35
3.3.8 三維輪廓儀 36
3.3.9 紫外光/可見光分光光譜儀 36
3.3.10 輝度量測系統 38
3.4 實驗藥品 38
第 四 章 實驗結果與討論 39
4.1 以機械均質法製備散射膜 41
4.1.1 表面改質劑的影響 41
4.1.2 超音波震盪的影響 44
4.2 以球磨法製備散射膜 47
4.2.1 ZrO2濃度的影響 47
4.2.2鋯珠尺寸的影響 54
4.2.3 二段球磨時間的影響 60
4.2.4 球磨後超音波震盪的影響 66
4.3 以稀釋的散射膜母液製備散射膜 72
4.3.1 ZrO2濃度的影響 73
4.3.2 散射膜厚度的影響 79
4.3.3 分散方式的影響 86
4.3.4 三段球磨時間的影響 92
結論 101
未來工作 103
參考文獻 105

[1]A. H. Eldin, M. Refaey, A. Farghly, “A Review on Photovoltaic Solar Energy Technology and its Efficiency.” 17th International Middle-East Power System Conference , Mansoura University, Egypt (2015)

[2]G. Azzouzi, W. Tazibt, “Improving Silicon Solar Cell Efficiency by Using the Impurity Photovoltaic Effect,” Energy Procedia, Vol. 41 (2013), pp.40-49

[3]S. Hore, C. Vetter, R. Kern, H. Smit, A. Hinsch, “Influence of scattering layers on efficiency of dye-sensitized solar cells,” Solar Energy Materials and Solar Cells, Vol. 90 (2006), pp.1176-1188

[4]C. S. Chou, M. G. Guo, K. H. Liu, Y. S. Chen, “Preparation of TiO2 particles and their applications in the light scattering layer of a dye-sensitized solar cell,” Applied Energy, Vol. 92 (2012), pp.224-233

[5]S. Kunic, Z. Sego, “OLED technology and displays,” 54th International Symposium ELMAR-2012, Zadar, Croatia (2012)

[6]S. H. Lee, D. S. Jo, B. S. Kim, D. H. Yoon, H. Chae, H. K. Chung, S. M. Cho, “Hybrid color-conversion layers for white emission from fluorescent blue organic light-emitting diodes,” Current Applied Physics, Vol. 17 (2017), pp.1108-1113

[7]D. Luo, Q. Chen, B. Liu, Y. Qiu, “Emergence of Flexible White Organic Light-Emitting Diodes,” Polymers, Vol. 11 (2019), Article.384

[8]S. M. Jeong, H. Takezoe, “Effect of Photonic Structures in Organic Light-Emitting Diodes - Light Extraction and Polarization Characteristics,” Organic Light Emitting Devices, (2012), Chapter.4

[9]T. Yamasaki, K. Sumioka, T. Tsutsui, “Organic light-emitting device with an ordered monolayer of silica microspheres as a scattering medium,” Applied Physics Letters, Vol. 76 (2000), pp.1243-1245

[10]C. H. Shin, E. Y. Shin, M. H. Kim, J. H. Lee, and Y. Choi, “Nanoparticle scattering layer for improving light extraction efficiency of organic light emitting diodes,” Optics Express, Vol. 23 (2015), pp.133-139

[11]M. K. Wei, H. Y. Lin, J. H. Lee, K. Y. Chen, Y. H. Ho, C. C. Lin, C. F. Wu, H. Y. Lin, J. H. Tsai, T. C. Wu, “Efficiency improvement and spectral shift of an organic light-emitting device with a square-based microlens array,” Optics Communications, Vol. 281 (2008), pp.5625-5632

[12]B. J. Matterson, J. M. Lupton, A. F. Safonov, M. G. Salt, W. L. Barnes, I. D. W. Samuel, “Increased Efficiency and Controlled Light Output from a Microstructured Light-Emitting Diode,” Advanced Materials, Vol. 13 (2001), pp.123-127

[13]Z. Y. Gao, Z. L. Wu, X. M. Li, J. L. Chang, D. P. Wu, P. F. Ma, F. Xu, S. Y. Gao, K. Jiang, “Application of hierarchical TiO2 spheres as scattering layer for enhanced photovoltaic performance in dye sensitized solar cell,” CrystEngComm, Vol. 15 (2013), pp.3351-3358

[14]J. L. Xu, K. Fan, W. Y. Shi, K. Li, T. Y. Peng, “Application of ZnO micro-flowers as scattering layer for ZnO-based dye-sensitized solar cells with enhanced conversion efficiency,” Solar Energy, Vol. 101 (2014), pp.150-159

[15]G. Syrrokostas, G. Leftheriotis, S. N. Yannopoulos, “Double-Layered Zirconia Films for Carbon-Based Mesoscopic Perovskite Solar Cells and Photodetectors,” Journal of Nanomaterials, Vol. 2019 (2019), Article.8348237

[16]R. Bathelt, D. Buchhauser, C. Gaditz, R. Paetzold, P. Wellmann, “Light extraction from OLEDs for lighting applications through light scattering,” Organic Electronics, Vol. 8 (2007), pp.293-299

[17]C. Y. Park, B. Choi, “Enhanced Light Extraction from Bottom Emission OLEDs by High Refractive Index Nanoparticle Scattering Layer,” Nanomaterials, Vol. 9 (2019), 1241

[18]李嘉甄, “分散技術與應用,” 工業材料雜誌, Vol. 360 (2016), pp.66-73

[19]H. Kamiya, M. Iijima, “Surface modification and characterization for dispersion stability of inorganic nanometer-scaled particles in liquid media,” Science and Technology of advanced materials, Vol. 11 (2010), 044304

[20]J. S. Kang, C. L. Yu, F. A. Zhang, “Effect of Silane Modified SiO2 Particles on Poly(MMA-HEMA) Soap-free Emulsion Polymerization,” Iranian Polymer Journal, Vol. 18 (2009), pp.927-935

[21]K. Anand, S. Varghese, T. Kurian, “Preparation of ultra-fine dispersions of zinc oxide by simple ball-milling : Optimization of process parameters,” Powder Technology, Vol. 271 (2015), pp.187-192

[22]K. Sato, J. G. Li, H. Kamiya, T. Ishigaki, “Ultrasonic Dispersion of TiO2 Nanoparticles in Aqueous Suspension,” Journal of the American Ceramic Society, Vol. 91 (2008), pp.2481-2487

[23]段啟聖, 張信貞, “噴墨用二氧化鈦微力研磨分散技術,” 工業材料雜誌, Vol. 360 (2016), pp.88-95

[24]https://www.keyence.com.tw/ss/products/microscope/roughness/

[25]https://www.renishaw.com/cmmsupport/knowledgebase/en/surface-finish-measurement--22135

[26]http://www.fsvs.ks.edu.tw/ezfiles/1/1001/img/62/175363261.pdf

[27]https://www.hi-top.com.tw/ITO%20SYSTEM/ITO%20MFS-630-TR.pdf

[28]https://zh.wikipedia.org/wiki/%E8%A7%86%E9%94%A5%E7%BB%86%E8%83%9E

[29]https://www.telescope-optics.net/eye_spectral_response.htm

[30]https://www.ledtronics.com/html/1931ChromaticityDiagram.htm