本實驗乃利用Si3N4來取代SiO2作為漸變折射層材料（Reflective Index-gradient Material）並結合圖樣化藍寶石基板（Patterned Sapphire Substrate, PSS）技術來製備新型圖樣化基板應用於氮化鎵發光二極體（GaN-based LED）作效率提升之探討。此技術主要是藉由氮化鎵的水平式成長來降低缺陷密度並以漸變折射層及圖樣化基板來提升光萃取效率。從模擬結果可得知，相較於PSS-LED，使用了Si3N4作為漸變折射層的發光二極體其光萃取效率約提升62.7%。由TEM圖可觀察到貫穿差排（Threading Dislocation）出現於基板溝渠處，而圖樣化基板上方則因為水平式磊晶生成了疊層缺陷（Stacking Fault）以及磊晶縫合時所形成的單一貫穿差排，實驗結果也證實了氮化鎵確實是以水平式的方式作磊晶。
  此外，經由實驗發現因為Si3N4粗糙表面導致氮化鎵經水平式成長後於氮化鎵與圖樣化基板間存在著氣體孔洞，根據模擬結果發現氣體孔洞的存在會影響到元件的發光效率。分別以Snell’s Law以及不同點光源的位置作分析可獲得四個不同結構之發光二極體其光萃取效率大小分別為PSN-LED > PSA-LED > PSO-LED > PSS-LED。

We use silicon nitride (Si3N4) to replace silicon dioxide (SiO2) as the reflective index-gradient material to fabricate GaN-based patterned sapphire substrate light-emitting diodes. It can not only reduce the threading dislocations densities but also enhance the light extraction efficiency (LEE). From the simulation results, the light extraction efficiency enhance approximate 62.7% higher than the PSS-LED. The TEM images show the threading dislocations exist on the trench region and stacking faults produce on the top of the pattern because of the GaN growth laterally. And also we found one threading dislocation which induced from coalescence of GaN thin film on the pattern region only. These evidences prove that the GaN film indeed was grown laterally.
  After re-growing, we observed the air voids exist on the top of the textured Si3N4 layer which were due to the GaN epitaxial lateral overgrowth. According to the simulation result, it reveals that the air voids will affect the final luminous efficiency. The luminous efficiency ranking of the four different LEDs is PSN-LED > PSA-LED > PSO-LED > PSS-LED.

目錄
致謝 ........................................................................................................ V
目錄 ....................................................................................................... VI
圖目錄 ................................................................................................ IXX
表目錄 ................................................................................................ XIII
第一章 序論 ........................................................................................... 1
1.1 前言 ........................................................................................... 1
1.2 發光二極體之發展 .................................................................... 5
1.3 圖樣化藍寶石基板發光二極體簡介 ......................................... 8
1.4 圖樣化藍寶石基板技術之文獻回顧 ......................................... 9
1.5 研究動機與目的 ...................................................................... 14
第二章 圖樣化藍寶石技術之介紹與應用 .......................................... 19
2.1 藍寶石基板之材料特性 .......................................................... 19
2.2 氮化鎵磊晶與差排理論 .......................................................... 22
2.2.1 貫穿差排之形成機制 .................................................... 23
2.2.2 差排對元件之影響 ........................................................ 24
2.3 圖樣化藍寶石基板對發光二極體量子效率之影響 ............... 25
2.4 濕式蝕刻製作圖樣化藍寶石基板之優缺點 ........................... 27
VII
2.5 漸變折射率 .............................................................................. 29
第三章 實驗方法與架構 ...................................................................... 32
3.1 圖樣化藍寶石基板之製備 ...................................................... 32
3.2 發光二極體元件之製作 .......................................................... 36
3.3製程儀器及原理 ....................................................................... 37
3.3.1電漿輔助化學氣相沉積系統 .......................................... 37
3.3.2高密度活性離子蝕刻系統 .............................................. 38
3.3.3 有機金屬化學氣相沉積系統 ......................................... 39
3.3.4 電子槍及熱蒸鍍系統 .................................................... 41
3.4 量測儀器與原理 ...................................................................... 41
3.4.1 場發射鎗掃描式電子顯微鏡 ......................................... 41
3.4.2 穿透式電子顯微鏡 ........................................................ 42
3.4.3 光激發螢光光譜 ............................................................ 44
3.4.4 L-I-V系統 ....................................................................... 45
第四章 結果分析與討論 ...................................................................... 48
4.1 漸變折射層之PSS-LED光學模擬結果與分析 ..................... 48
4.2 具有氣體孔洞之圖樣化藍寶石基板發光二極體之製備 ........ 53
4.2.1 以活性離子蝕刻製備表面粗糙之圖樣化氮化矽 .......... 53
4.2.2 以濕式蝕刻製備圖樣化藍寶石基板 ............................. 55
VIII
4.3 具有氣體孔洞之圖樣化藍寶石基板發光二極體結果分析 .... 58
4.3.1 掃描式電子顯微鏡分析 ................................................. 59
4.3.2 穿透式電子顯微鏡分析 ................................................. 60
4.3.3 變溫PL量測分析 .......................................................... 63
4.3.4 光學模擬結果與分析 .................................................... 66
第五章 結論與未來工作 ...................................................................... 71
5.1 結論 ......................................................................................... 71
5.2 未來工作.................................................................................. 72
參考文獻 ............................................................................................... 73
IX
圖目錄
圖1.1 發光二極體之發光原理 ............................................................. 2
圖1.2 直接能隙與間接能隙比較圖 ..................................................... 2
圖1.3 Ⅲ-V族氮化物能隙與晶格常數之關係圖 ................................. 3
圖1.4半導體材料之能隙發光光譜圖 .................................................. 3
圖1.5 提升發光二極體效率之各種製程方式 ...................................... 7
圖1.6 圖樣化藍寶石基板結構示意圖 ................................................. 8
圖1.7氣體孔洞示意圖 ........................................................................ 14
圖1.8 Wurtzite結構示意圖 .............................................................. 15
圖1.9 氮化鎵之（0001）面與Sapphire之（0001）面原子排列關係............................................................................................................... 15
圖1.10內部全反射示意圖 .................................................................. 16
圖2.1 藍寶石的晶體結構 ................................................................... 20
圖2.2藍寶石之蝕刻晶面結構 (a)俯視圖 (b)側視圖 ..................... 20
圖2.3 (a) 邊緣差排(b) 螺旋差排 ................................................... 24
圖2.4 電子與電洞之輻射結合 ........................................................... 25
圖2.5 圖樣化藍寶石基板磊晶的示意圖與不同深度圖樣化藍寶石基板磊晶之TEM 圖 .................................................................................. 26
圖2.6 圖樣化藍寶石基板光萃取示意圖 ........................................... 27
X
圖2.7 (a)蝕刻前：塗佈光阻 (b)定義圖型 (c)濕式蝕刻與底切情形............................................................................................................... 28
圖2.8 濕式蝕刻過程示意圖 ............................................................... 28
圖2.9 (a) 疏→密之折射現象 (b) 密→疏之折射現象 .................. 31
圖3.1 圖樣化藍寶石基板之製作流程示意圖 .................................... 35
圖3.2圖樣化藍寶石之氮化鎵磊晶結構 ............................................ 37
圖3.3電漿輔助化學氣相沉積系統 .................................................... 38
圖3.4介電材料活性離子蝕刻系統 .................................................... 39
圖3.5有機金屬化學氣相沉積法反應原理示意圖 ............................. 40
圖3.6有機金屬化學氣相沉積系統 .................................................... 40
圖3.7 電子槍及熱蒸鍍系統 ............................................................... 41
圖3.8 場發射鎗掃描式電子顯微鏡系統 ........................................... 42
圖3.9 明/暗視野原理示意圖 ............................................................. 43
圖3.10 穿透式電子顯微鏡系統 ......................................................... 44
圖3.11 電子躍遷示意圖 ..................................................................... 45
圖3.12 L-I-V量測系統 ...................................................................... 47
圖4.1 光學模擬模型 ...............................................................................
(a) CSS-LED (b) PSS-LED (c) PSN-LED (d) PSO-LED ................... 49
圖4.2 偵測器收光方式示意圖 ........................................................... 50
圖4.3 偵測器全收光之模擬結果 ....................................................... 51
XI
圖4.4 偵測器(a)上收光 (b)下收光之模擬結果 .............................. 52
圖4.5 PSS-110經活性離子蝕刻120 s後之SEM圖 .............................
(a) top view (b) cross section .................................................... 54
圖4.6 PSS-220經活性離子蝕刻220 s後之SEM圖 .............................
(a) top view (b) cross section .................................................... 54
圖4.7 PSS-330經活性離子蝕刻260 s後之SEM圖 .............................
(a) top view (b) cross section .................................................... 54
圖4.8為PSS-110在溫度260℃下經硫磷酸混合液蝕刻4.5 min後之SEM圖(a) top view (b) cross section (c) tilt 30o ................. 56
圖4.9為PSS-220在溫度260℃下經硫磷酸混合液蝕刻4.5 min後之SEM圖(a) top view (b) cross section (c) tilt 30o ................. 57
圖4.10為PSS-330在溫度260℃下經硫磷酸混合液蝕刻4.5 min後之SEM圖(a) top view (b) cross section (c) tilt 30o .................................... 58
圖4.11 PSS-110磊晶後之cross-sectional SEM圖 ....................... 59
圖4.12 PSS-220磊晶後之cross-sectional SEM圖 ....................... 60
圖4.13 PSS-330磊晶後之cross-sectional SEM圖 ....................... 60
圖4.14 PSS-330之STEM圖 ................................................................ 61
圖4.15 PSS-330暗視野之TEM圖(a) 6 KX (b) 12 KX ................... 62
圖4.16 PSS-330明視野之TEM圖(a) 6 KX (b) 12 KX ................... 62
XII
圖4.17 PSS-110之變溫PL光譜圖 .................................................... 63
圖4.18 PSS-220之變溫PL光譜圖 .................................................... 64
圖4.19 PSS-330之變溫PL光譜圖 .................................................... 64
圖4.20 四種不同圖樣化結構之模擬結果.......................................... 68
圖4.21 光線路徑示意圖 (a) CSS (b) PSS (c) 漸變折射層 (d) 中間層折射率小於Sapphire ................................................................... 68
圖4.22點光源設置位置(a) between (b) center (c) edge ......... 70
圖4.23 點光源模擬結果 ..................................................................... 70
XIII
表目錄
表1.1 LED照明應用領域及優點 ....................................................... 4
表1.2 圖樣化藍寶石基板之相關文獻 ................................................ 10
表2.2 單晶型態之藍寶石材料基本物性 ............................................ 21
表4.1 光學模擬之建模條件 ................................................................ 50

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