臺灣博碩士論文加值系統

以射頻磁控濺鍍法(Radio Frequency Magnetron Sputtering)製備氧化鋅(ZnO)為基底的透明導電薄膜已經被廣泛應用於各種光電元件。本研究以射頻磁控濺鍍系統沉積鎂氟共摻雜氧化鋅薄膜(MFZO)以及氟摻雜氧化鋅薄膜(FZO)於玻璃基板上。濺鍍靶材以自行壓製摻雜量為3 mol%之MgF2與ZnF2的氧化鋅濺鍍靶材，以改變濺鍍之基板溫度、快速熱退火之溫度及時間於真空中進行快速熱退火處理，研究濺鍍參數以及快速熱退火處理對於MFZO與FZO薄膜之結構、表面形貌、光電特性及組成成分的影響。再使用稀鹽酸溶液蝕刻薄膜表面，最後使用電漿增強式化學氣相沉積法(PECVD)沉積p-i-n結構的氫化非晶矽薄膜太陽電池(α-Si:H SCs)，以探討薄膜製程對太陽電池之光電轉換效率的影響。
基板溫度由室溫至200℃沉積時，MFZO及FZO薄膜在基板溫度200℃具有最佳的電阻率，分別為1.18×10-3 Ω-cm、8.57×10-4 Ω-cm，而光學能隙分別為3.803 eV以及3.79 eV。改變快速熱退火溫度由300至500℃及快速熱退火時間15至120 s後，MFZO及FZO薄膜在溫度400℃及時間30 s時有最佳的電阻率分別為1.30×10-3 Ω-cm、7.96×10-4 Ω-cm，並且在可見光區的平均穿透率皆約為93%，光學能隙分別為3.812 eV以及3.831 eV，FOM分別為1.18×10-2 Ω-1以及1.99×10-2 Ω-1。而在所有薄膜經由稀鹽酸蝕刻後，片電阻皆上升。改變稀鹽酸濃度由0.5%至0.7%，室溫沉積薄膜於濃度0.5%時有最佳FOM。基板溫度200℃之MFZO及FZO蝕刻後薄膜，在可見光區的最佳平均霧度分別為55.1%及42.3%。
在太陽電池的部分，稀鹽酸蝕刻MFZO薄膜表面後，太陽電池短路電流密度7.281 mA/cm2、開路電壓0.882 V、填充因子68.77%、轉換效率4.418%。與未蝕刻之MFZO薄膜相比，可提升太陽電池約12 %短路電流密度、13.7%填充因子、3.1%開路電壓以及34.1%轉換效率。相對稀鹽酸蝕刻FZO薄膜太陽電池短路電流密度7.217 mA/cm2、開路電壓0.869 V、填充因子64.55%、轉換效率4.05%，以MFZO薄膜為透明電極的太陽電池效能較好。

ZnO-based transparent conducting thin films prepared by radio frequency (RF) magnetron sputtering have been widely used in various optoelectronic devices. In this study, a magnesium-fluorine co-doped zinc oxide film (MFZO) and a fluorine-doped zinc oxide film (FZO) were deposited on glass substrates by a RF magnetron sputtering system. The sputtering targets are with zinc oxide targets containing 3 mol% of MgF2 and ZnF2, respectively. Effects of substrate temperature, rapid thermal annealing (RTA) temperature and time were investigated on structural, surface morphological, electrical, optical, and composition properties of those films. Hydrogenated amorphous silicon thin films solar cells (α-Si:H SCs) were prepared by plasma enhanced chemical vapor deposition to investigate the influence of the TCO films on efficiency of the solar cells. When the substrates temperature varied from room temperature to 200 ℃, the MFZO and FZO films had an optimum resistivity of 1.18×10-3 Ω-cm and 8.57×10-4 Ω-cm at a substrate temperature of 200 ℃, respectively, and the optical band gap were 3.803 eV and 3.790 eV, respectively. After RTA treatment at temperatures of 300 to 500 ℃ and at times of 15 to 120 s, MFZO and FZO films had optimum resistivities of 1.30×10-3 Ω-cm and 7.96×10-4 Ω-cm, respectively, at an RTA temperature of 400 ℃ for 30 s. The average transmittance in the visible region were both about 93%, the optical band gaps were 3.812 eV and 3.831 eV, respectively, and the FOM were 1.18×10-2 Ω-1 and 1.99×10-2 Ω-1, respectively. These films deposited at room temperature were etched through dilute hydrochloric acid concentration of 0.5% to 0.7%, and the optimum FOM was obtained at 0.5%. The average haze ratio of the etched MFZO and etched FZO films at a substrate temperature of 200 ℃ in the visible region is 55.1% and 42.3%, respectively.
As to the p-i-n α-Si:H SCs prepared on the etched MFZO film, the short-circuit current density, the open circuit voltage, the fill factor, and the efficiency were 7.281 mA/cm2, 0.882 V, 68.77%, and 4.418%, respectively. Compared with the unetched MFZO electrode, it can increase the solar cells 12% short-circuit current density, 13.7% fill factor, 3.1% open circuit voltage and 34.1% efficiency. However, α-Si:H SCs prepared on the etched FZO film achieved the short-circuit current density, the open circuit voltage, the fill factor, and the efficiency of 7.217 mA / cm2, 0.869 V, 64.55%, and 4.05%, respectively. We conclude that α-Si:H SCs with the MFZO front electrode have better performance than those with the FZO one.

致謝 .................................................................................................................. i
摘要 ............................................................................................................... iii
Abstract .......................................................................................................... iv
目錄 ................................................................................................................ vi
圖目錄 ............................................................................................................. x
表目錄 .......................................................................................................... xiv
第一章 緒論 ........................................................................................... 1
1.1 前言 ................................................................................................... 1
1.2 研究動機與目的 ............................................................................... 1
第二章 文獻回顧與基礎理論 .............................................................. 5
2.1 文獻回顧 ........................................................................................... 5
2.2 基礎理論 ........................................................................................... 6
2.2.1 氧化鋅之晶體結構與特性 .................................................... 6
2.2.2 共摻雜鎂氟之氧化鋅(MFZO)薄膜 ...................................... 8
2.2.2.1 電學性質 .................................................................... 8
2.2.2.2 光學性質 .................................................................... 9
2.2.3 電漿基礎原理 ...................................................................... 12
2.2.4 射頻磁控濺鍍 ...................................................................... 13
2.2.4.1 濺鍍原理 ................................................................... 13
2.2.4.2 直流與射頻濺鍍 ....................................................... 14
2.2.4.3 磁控濺鍍 ................................................................... 15
2.2.5 薄膜沉積 .............................................................................. 15
2.2.5.1 薄膜成長機制 ........................................................... 15
2.2.5.2 Thorton 模型 ............................................................ 17
2.2.6 薄膜快速熱退火處理 .......................................................... 18
2.2.7 氫化非晶矽(α-Si:H)薄膜太陽電池 .................................... 18
2.2.7.1 太陽電池 ................................................................... 18
2.2.7.2 電漿增強式化學氣相沈積法 ................................... 21
第三章 實驗步驟與方法 ..................................................................... 22
3.1 實驗製程與流程分析 ..................................................................... 22
3.2 靶材製作流程 ................................................................................. 23
3.2.1 靶材粉末調製 ..................................................................... 23
3.2.2 靶材製程 ............................................................................. 24
3.3 基板切割與清洗流程 ..................................................................... 25
3.4 透明導電薄膜沉積 ......................................................................... 26
3.4.1 薄膜沉積設備 ..................................................................... 26
3.4.2 鎂氟共摻雜之氧化鋅(MFZO)薄膜製程參數 ................... 26
3.5 薄膜快速熱退火製程 .................................................................... 27
3.5.1 薄膜快速熱退火設備 .......................................................... 27
3.5.2 薄膜快速熱退火參數 .......................................................... 28
3.6 薄膜化學濕蝕刻製程與參數 ......................................................... 28
3.7 太陽電池沉積 ................................................................................. 29
3.7.1 太陽電池沉積設備 .............................................................. 29
3.7.2 氫化非晶矽薄膜太陽電池(α-si:H TFSC)製程參數 .......... 29
3.8 太陽電池背電極製程設備與參數 ................................................. 30
3.9 薄膜量測分析 ................................................................................. 31
3.9.1 薄膜結構分析 ..................................................................... 31
3.9.1.1 薄膜SEM 厚度量測 ................................................ 31
3.9.1.2 薄膜XRD 結構分析 ................................................ 31
3.9.1.3 薄膜SEM 表面形貌分析 ........................................ 32
3.9.1.4 薄膜AFM 表面粗糙度分析 .................................... 32
3.9.2 薄膜電性量測 ...................................................................... 33
3.9.2.1 薄膜片電阻量測 ....................................................... 33
3.9.2.2 薄膜霍爾效應量測 ................................................... 33
3.9.3 薄膜光學量測 ...................................................................... 34
3.9.4 薄膜元素成分分析 .............................................................. 35
3.9.4.1 薄膜元素鍵結分析 ................................................... 35
3.9.4.2 薄膜元素縱深分析 .................................................. 36
3.10 太陽電池量測分析 ....................................................................... 36
3.10.1 太陽電池電性與效率量測 ................................................ 36
3.10.2 太陽電池外部量子效率量測 ............................................ 36
第四章 結果與討論 ............................................................................. 37
4.1 濺鍍製程參數對薄膜的影響 ......................................................... 37
4.1.1 沉積溫度對於薄膜特性之影響 ......................................... 37
4.1.1.1 薄膜沉積速率 .......................................................... 37
4.1.1.2 薄膜結構XRD 分析 ............................................... 38
4.1.1.3 薄膜形貌SEM 分析 ............................................... 41
4.1.1.4 薄膜粗糙度AFM 分析 ........................................... 43
4.1.1.5 薄膜電性Hall effect 分析 ....................................... 45
4.1.1.6 薄膜電性穩定性分析 .............................................. 47
4.1.1.7 薄膜光學分析 .......................................................... 48
4.1.1.8 薄膜FOM ................................................................. 52
4.1.1.9 薄膜XPS 分析 ......................................................... 53
4.1.10 薄膜SIMS 分析 ........................................................ 61
4.2 快速熱退火處理對於MFZO 薄膜之影響 .................................. 64
4.2.1 不同RTA 的溫度對於薄膜特性之影響 ............................ 64
4.2.1.1 不同RTA 的溫度之薄膜XRD 分析 ...................... 64
4.2.2.2 不同RTA 的溫度之薄膜SEM 分析 ...................... 66
4.2.2.3 不同RTA 的溫度之薄膜AFM 分析 ..................... 67
4.2.2.4 不同RTA 的溫度之薄膜電性分析 ........................ 68
4.2.2.5 快速熱退火後薄膜電性穩定性分析 ...................... 71
4.2.2.6 不同RTA 的溫度之薄膜光學分析 ........................ 72
4.2.2 不同RTA 的時間對於薄膜特性之影響 ............................ 76
4.2.2.1 不同RTA 的時間之薄膜XRD 分析 ....................... 76
4.2.2.2 不同RTA 的時間之薄膜電性分析 ......................... 78
4.2.2.3 不同RTA 的時間之薄膜光學分析 ......................... 81
4.2.2.4 快速熱退火後XPS 分析 ........................................ 84
4.2.2.5 快速熱退火後SIMS 分析 ....................................... 90
4.3 鹽酸濕蝕刻對薄膜的影響 ............................................................. 92
4.3.1 薄膜濕蝕刻前之特性 .......................................................... 92
4.3.1.1 蝕刻前薄膜SEM 形貌 ............................................ 92
4.3.1.2 蝕刻前薄膜之電性 ................................................... 93
4.3.1.3 蝕刻前薄膜之光學特性 ........................................... 94
4.3.2 不同鹽酸濃度蝕刻對薄膜的影響 ...................................... 97
4.3.2.1 不同鹽酸濃度蝕刻薄膜之蝕刻速率 ..................... 97
4.3.2.2 不同鹽酸濃度蝕刻前後SEM 形貌分析 ............... 98
4.3.2.3 不同鹽酸濃度蝕刻薄膜前後電性分析 ............... 101
4.3.2.4 不同鹽酸濃度濕蝕刻光學分析............................ 102
4.3.3 相同鹽酸濃度蝕刻不同製程薄膜的影響....................... 106
4.3.3.1 相同濃度鹽酸蝕刻薄膜之蝕刻速率 .................... 106
4.3.3.2 薄膜蝕刻後SEM 形貌 .......................................... 107
4.3.3.3 相同濃度鹽酸濕蝕刻薄膜之片電阻電性量測 .... 109
4.3.3.4 相同鹽酸濃度濕蝕刻薄膜光學分析 ................... 110
4.4 應用於氫化非晶矽薄膜太陽電池 .............................................. 115
4.4.1 氫化非晶矽薄膜太陽電池之結構 ................................... 115
4.4.2 太陽電池之外部量子效率 ............................................... 116
4.4.3 太陽電池光電效率量測 ................................................... 117
第五章 結論 ....................................................................................... 119
參考文獻 ..................................................................................................... 121

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