本論文利用溶膠-凝膠法 (Sol-Gel) ，以矽酸四乙酯（TEOS）為前驅物，藉由調配溫度、氨水、去離子水比例，合成不同粒徑之二氧化矽球體，並利用場發掃描式電子顯微鏡 (FE-SEM) 及粒徑分析儀觀測二氧化矽球體尺寸及分佈狀況，並利用田口方法建立各因子對球體粒徑之影響，進而求得最佳值。利用合成之二氧化矽球體做為遮罩並藉由乾式蝕刻方式進行發光二極體表面粗化，以達提升發光二極體出光效率之目的。表面粗化實驗配合探討各蝕刻深度，對於發光二極體表面粗化製程之影響，本實驗所探討之因子為球徑大小80nm、塗佈速度(500~4000rpm) 及蝕刻深度(50~140nm)。結果發現，此三項因子對於光致螢光之強度皆有顯著影響，且在塗佈速度為1500rpm、蝕刻深度為100nm 時會有最佳光致螢光之強度值1.78×107。經研究發現實驗結果與理論相符合，與表面未粗化之發光二極體相比，最佳粗化條件下，其出光效率可增加達90%。

In this study, we synthesize a variety of sizes of SiO2 nano-spheres from the precursor of TEOS, with varied ratio of temperature, deionized water, ammonia aqua by the sol-gel method, we obtain the optimal value of the model established by the response taguchi method. The sizes and the distribution condition of SiO2 nano-spheres on are observed by field emission gun scanning electron microscopy (FE-SEM) and particle analyzer. Further, we apply SiO2 nano-spheres as a hard mask to obtain patterned and roughing surface on the LED-Epitaxy wafer, and the increases light extraction efficiency of LED. Those parametric factors for the experiment of roughing wafer surface are sphere dimension, 80nm, spin-coated rotation speed, 500~4000rpm, and etching depth, 50~140nm, respectively. From the roughen method, three above-mentioned factors possess obvious of influence on the Photoluminescence intensity. The optimized value of the Photoluminescence intensity from calculation is 1.78×107 while these values, 80nm, 1500rpm, and 100nm are being designated for the three corresponding factors. Under the optimized roughen condition, the light extraction efficiency of roughen LED sample increases up to 90% in comparison with non-roughen LED sample.

中文摘要 ........................................................................................................................... i
Abstract ............................................................................................................................. ii
目錄 ................................................................................................................................. iii
圖目錄 .............................................................................................................................. v
表目錄 ............................................................................................................................ vii

第一章前言 .................................................................................................................... 1
1-1 溶膠-凝膠法之介紹 .......................................................................................... 1
1-2 GaN 材料特性 .................................................................................................... 2
1-3 發光二極體現況與研究動機 ........................................................................... 2
1-4 微小球體應用於發光二極體之介紹 ............................................................... 3
1-5 研究動機 ........................................................................................................... 4

第二章文章回顧與理論基礎 ........................................................................................ 6
2-1 二氧化矽球體製備 ........................................................................................... 6
2-1-1 溶膠-凝膠法之反應機制理論 .............................................................. 6
2-1-2 二氧化矽的成核及成長機制 ................................................................ 9
2-1-3 製備參數對奈米二氧化矽之影響 ...................................................... 10
2-2 LED 原理與介紹 ............................................................................................. 13
2-2-1 LED 發光效率 ...................................................................................... 14
2-3 奈米球體乾式蝕刻之應用 ............................................................................. 15
2-3-1 奈米球體微縮製程 .............................................................................. 15
2-3-2 奈米球體應用於LED 表面粗糙化 .................................................... 15
2-4 田口方法之基本原理 ..................................................................................... 17
2-4-1 田口實驗計畫法介紹 .......................................................................... 18

第三章實驗步驟與分析儀器 ...................................................................................... 28
3-1 實驗設計變因 ................................................................................................. 28
3-2 實驗試藥 ......................................................................................................... 28
3-3 儀器介紹 ......................................................................................................... 29
3-3-1 實驗儀器介紹 ...................................................................................... 29
3-3-2 分析儀器介紹 ...................................................................................... 30
3-4 實驗步驟 ......................................................................................................... 30
3-4-1 溶膠-凝膠法二氧化矽球體之製備 .................................................... 30
3-4-2 田口方法實驗法設計 .......................................................................... 30
3-4-3 LED 之結構設計 .................................................................................. 31
3-4-4 表面粗糙化流程 .................................................................................. 31
3-5 分析儀器量測原理 ......................................................................................... 32
3-5-1 場發射掃描式電子顯微鏡(FE-SEM) ................................................. 32
3-5-2 粒徑與表面電位分析儀(Zetasizer) .................................................... 32
3-5-3 光致發光光譜儀(PL) .......................................................................... 32

第四章結果與討論 ...................................................................................................... 44
4-1 田口方法設計於二氧化矽球體之合成 ......................................................... 44
4-2 二氧化矽球體合成之參數 ............................................................................. 45
4-2-1 反應溫度的影響 .................................................................................. 45
4-2-2 TEOS 含量的影響 ................................................................................ 45
4-2-3 NH3 含量的影響 ................................................................................... 46
4-2-4 H2O 含量的影響 ................................................................................... 46
4-3 二氧化矽球體應用於LED 表面粗糙化之參數 ........................................... 47
4-3-1 旋轉塗佈速度以及時間之影響 .......................................................... 47
4-3-2 二氧化矽球體蝕刻深度的影響 .......................................................... 48
4-3-3 二氧化矽球體微縮的影響 .................................................................. 48

第五章結論 .................................................................................................................. 69
參考文獻 ........................................................................................................................ 71

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