臺灣博碩士論文加值系統

CIGS（硒化銅銦鎵）薄膜型太陽能電池，有著高吸收係數的特性，因此在能源問題浮現的現代，備受大家關注。本文針對CIGS薄膜之不同堆疊製程進行研究探討，先以直流濺鍍法將Mo薄膜沈積於不鏽鋼基材上，再利用三明治堆疊法(In/CuGa/In)沈積CuGa及In作為前驅物層，再以高溫爐進行三階段硒化，使前驅物與Se結合形成CIGS吸收層。並探討不同堆疊方式的前驅物製程對CIGS的影響，然後將沈積好的薄膜，先以SEM電子顯微鏡及X光能譜分析儀觀看表面結構及成份分析，接著以3D表面輪廓儀量測表面粗造度，再以X光繞射儀量測晶體結構強度。緩衝層是以原子束蒸鍍機製備ZnS薄膜再量測光穿透率，透明導電層是以濺鍍機以及ALD進行AZO薄膜沈積，再量測光穿透率以及電性。最後是以三明治堆疊法(In 600 nm / CuGa 300 nm / In 600 nm)這組試片，Cu/(In+Ga) ratio (0.941)接近做為太陽能電池元件，晶體結構2θ約26.97 ∘的 ( 112 ) 波峰的晶體結構強度約59875(cps)是最佳的，緩衝層ZnS光穿透率最高為75.43%，透明導電層是以ALD製備的AZO光穿透率最高為85.46%，在量測電性方面，以In 600 nm / CuGa 300 nm / In 600 nm這組電性最佳。

CIGS thin films have become one of the most important absorption layer in solar cells because of its high efficiency. This work characterizes flexible CIGS solar cells synthesized with various deposition methods. The Mo conducting films is sputtered on stainless steel shells, and utilizes sandwich deposition method (In/CuGa/In) to sputter CIG precursor films on the Mo/stainless steel substrates. Then, the CIGS absorption layers are synthesized with three stage high temperature selenization. The surface roughness, micro structure, composition, crystallization, and conductivity of the CIGS are characterized by the 3D profiler, scanning electronic microscope, energy dispersive spectrometer, X-ray diffraction machine, and Hall effects meter. To finish the solar cell, the ZnS buffer layer and AZO transparently conductive layer are deposited on the CIGS film with E-beam evaporation, sputtering, and atomic layer deposition. The result shows that the specimen of In 600 nm/ CuGa 300 nm/ In 600 nm with Cu/(In+Ga) ratio 0.941 behaves the best photoelectric performance.

論文摘要 I
ABSTRACT II
致謝 III
目錄 IV
表目錄 XI
第一章　緒論 1
1.1　研究動機 1
1.2　研究背景 2
1.3 文獻回顧 4
1.3.1　Mo薄膜之基本特性及應用 4
1.3.2　CIGS 薄膜之基本特性及應用 5
1.3.3　CIGS吸收層之微結構及優選取向 6
1.3.4　緩衝層相關文獻回顧 8
1.3.5　透明導電膜相關文獻回顧 9
1.4　本文作法 10
第二章　基礎理論與研究方法 13
2.1　太陽能原理 13
2.1.1　太陽光譜 13
2.1.2　太陽能發展 13
2.1.3　半導體簡介 14
2.1.4　太陽能原理 16
2.2　濺鍍原理 18
2.3 原子層沈積原理 19
2.3.1 原子層化學氣相沈積之成長機制 21
2.3.2 溫度對於原子層沈積系統之影響 29
2.4　電子束蒸鍍機(evaporation chamber) 30
2.5　表面輪廓儀 (3D Profiler) 32
2.5.1　表面輪廓儀架構及原理 32
2.5.2　表面輪廓儀探針特性 33
2.5.3　表面輪廓儀量測時注意事項 33
2.5.4　表面輪廓儀實驗步驟 33
2.6　X光繞射儀 34
2.6.1 X光繞射儀架構 34
2.6.2　X光繞射儀原理 35
2.6.3　優選取向 36
2.6.4　晶粒大小計算 37
2.6.5　X光繞射儀量測時注意事項 39
2.6.6　X光繞射儀實驗步驟 39
2.7　X光能譜分析儀 39
2.7.1　X光能譜分析儀原理 40
2.7.2　X光能譜分析儀注意事項 40
2.7.3　X光能譜分析儀實驗步驟 41
2.8　光激發光譜儀 41
2.8.1　反射率架構與原理 41
2.8.2　反射率量測時注意事項 42
2.8.3　反射率實驗步驟 42
2.9　四點探針電阻儀 42
2.9.1　四點探針電阻儀原理 42
2.9.2　四點探針電阻儀量測注意事項 43
2.9.3　四點探針電阻儀實驗步驟 44
2.10　霍爾效應量測儀 44
2.10.1　霍爾效應量測儀架構與原理 44
2.10.2　霍爾效應量測時注意事項 45
2.10.3　霍爾效應量測儀實驗步驟 45
第三章　薄膜製作 46
3.1　基材選用 46
3.2　實驗材料 47
3.2.1　背電極材料 47
3.2.2　前驅物材料 48
3.2.3　硒化材料 48
3.3　鍍前處理 49
3.3.1　表面油汙處理 49
3.3.2　清潔液清洗 49
3.3.3　清除表面殘留溶劑 49
3.3.4　烘乾試片 49
3.4　實驗參數 50
3.4.1　實驗步驟 50
3.4.2　Mo初步分析 51
3.5　沈積前驅物薄膜 53
3.5.1　前驅物比面分析 54
3.5.2　前驅物成份分析 59
3.6　硒化 61
3.6.1　實驗步驟 61
第四章　結果與討論 64
4.1 表面結構分析 64
4.2 成份分析 68
4.3 表面粗糙度分析 72
4.4 CIGS薄膜之晶相分析 77
4.5 硫化鋅(ZnS)緩衝層鍍製 81
4.5.1 硫化鋅膜厚量測 82
4.5.2 硫化鋅光穿透率分析 84
4.6 透明導電層 (AZO)製作 84
4.6.1 AZO膜厚量測 86
4.6.2 AZO光穿透率分析 87
4.6.3 電特性分析 87
4.7 P-N接面檢測 88
4.8 正電極鋁金屬製作 94
4.9 日光燈模擬系統 95
第五章 結論 96

圖目錄
圖1-1 CIGS薄膜型太陽能電池示意圖 2
圖1-2 各種太陽能電池的效率演變圖(1975~2013) 4
圖1-3 體心立方結構 4
圖1-4 黃銅礦結構 6
圖1-5 SEM觀察CIGS薄膜不同 Ga/（In+ Ga）原子比之橫截面圖 7
圖1-6 CIGS在不同Ga/（In+ Ga）原子比之晶體結構強度圖 8
圖1-7 實驗流程圖 12
圖2-1　太陽能電池的原理圖[61] 17
圖2-2　太陽能電池暗電流與光電流之電壓特性曲線[29] 18
圖2-3 濺鍍示意圖 19
圖 2 4 ALD垂直式成長腔體示意圖 20
圖 2 5 ALD水平式成長腔體示意圖 20
圖 2 6 ALD之反應室 21
圖 2 7 原子層沈積系統示意圖 22
圖 2 8 原子層沈積四個步驟(1)前驅物引進(2)沖洗(3)反應物引進(4)沖洗 23
圖 2 9 一個循環時間等於兩種前驅物的脈衝時間加上兩個沖洗的時間 24
圖 2 10 Al2O3薄膜經由原子層沈積，均勻地覆蓋在HSG表面上 25
圖 2 11 TiN 薄膜均勻地覆蓋在25:1 高深寬比的深溝渠內 25
圖 2-12 氧化鋅摻鋁薄膜沈積示意圖 28
圖 2-13 氧化鋅摻鋁薄膜沈積總時間圖 29
圖 2 14 原子層沈積窗口，描述表面薄膜生長過程速率與溫度之關係圖 30
圖2-15 電子束蒸鍍機示意圖 31
圖2-16　表面輪廓儀量測示意圖 32
圖2-17　表面輪廓儀儀器架構示意圖 33
圖2-18　X光繞射儀架構 34
圖2-19　布拉格繞射原理 35
圖2-20　X-ray繞射量測方式 36
圖2-21　掃描式電子顯微鏡附加X光能譜分析儀 39
圖2-22　化學成份分析圖 40
圖2-23　量測反射率架構圖 41
圖2-24　四點探針電阻儀示意圖 43
圖2-25 霍爾效應量測儀架構圖 44
圖3-1　 不鏽鋼基材之外觀圖 46
圖3-2　 Mo濺鍍靶材之外觀圖 47
圖3-3　 CuGa、In濺鍍靶材之外觀圖 48
圖3-4 Se顆粒之外觀圖 48
圖3-5　 濺鍍機之外觀 50
圖3-6　 Mo / SS之表面粗糙度示意圖 52
圖3-7 Mo / SS之趨勢圖 52
圖3-8 實驗堆疊示意圖 54
圖3-9 Sample A之前驅物SEM表面結構圖 55
圖3-10 Sample B之前驅物SEM表面結構圖 55
圖3-11 Sample C之前驅物SEM表面結構圖 56
圖3-12 Sample D之前驅物SEM表面結構圖 56
圖3-13 Sample E之前驅物SEM表面結構圖 57
圖3-14 Sample F之前驅物SEM表面結構圖 57
圖3-15 Sample G之前驅物SEM表面結構圖 58
圖3-16 Sample H之前驅物SEM表面結構圖 58
圖3-17 Sample A、B成份分析示意圖 59
圖3-18 Sample C、D成份分析示意圖 59
圖3-19 Sample E、F成份分析示意圖 60
圖3-20 Sample G、H成份分析示意圖 60
圖3-21 硒化高溫爐示意圖 62
圖3-22 硒化三階段生溫曲線圖 63
圖4-1 Sample A之CIGS的 SEM表面結構圖 64
圖4-2 Sample B之CIGS的 SEM表面結構圖 65
圖4-3 Sample C之CIGS的 SEM表面結構圖 65
圖4-4 Sample D之CIGS的 SEM表面結構圖 66
圖4-5 Sample E之CIGS的 SEM表面結構圖 66
圖4-6 Sample F之CIGS的 SEM表面結構圖 67
圖4-7 Sample G之CIGS的 SEM表面結構圖 67
圖4-8 Sample H之CIGS的 SEM表面結構圖 68
圖4-9 Sample A、B成份分析示意圖 70
圖4-10 Sample C、D成份分析示意圖 70
圖4-11 Sample F、G成份分析示意圖 71
圖4-12 Sample G、H成份分析示意圖 71
圖4-13 Sample A 之CIGS表面粗糙度示意圖 72
圖4-14 Sample B 之CIGS表面粗糙度示意圖 73
圖4-15 Sample C 之CIGS表面粗糙度示意圖 73
圖4-16 Sample D 之CIGS表面粗糙度示意圖 74
圖4-17 Sample E 之CIGS表面粗糙度示意圖 74
圖4-18 Sample F 之CIGS表面粗糙度示意圖 75
圖4-19 Sample G 之CIGS表面粗糙度示意圖 75
圖4-20 Sample H 之CIGS表面粗糙度示意圖 76
圖4-21 Sample A、B、C、D、E、F、G、H粗糙度之趨勢圖 77
圖4-22 不同堆疊之 CIGS( Sample A、B、C、D )之( 112 )晶相分析示意圖 79
圖4-23 不同堆疊之 CIGS( Sample E、F、G、H ) 之 ( 112 )晶相分析示意圖 80
圖4-24 ZnS /glass 量測50 nm膜厚示意圖 81
圖4-25 ZnS /glass 量測透光率之示意圖 82
圖4-26 膜厚量測示意圖 82
圖4-27 膜厚量測示意圖 83
圖4-28 膜厚量測示意圖 83
圖4-29 膜厚量測示意圖 83
圖4-30 四組ZnS之透光率示意圖 84
圖4-31 AZO / Glass (ALD)量測500 nm之膜厚示意圖 86
圖4-32 AZO / Glass (Sputter)量測500 nm之膜厚示意圖 86
圖4-33 氧化鋅摻鋁薄膜沈積於Glass上之光穿透率 87
圖4-34 Sample A CIGS / MO / SS量測P-N示意圖 88
圖4-35 Sample B CIGS / Mo / SS量測P-N示意圖 89
圖4-36 Sample C CIGS / Mo / SS量測P-N示意圖 89
圖4-37 Sample D CIGS / Mo / SS量測P-N示意圖 90
圖4-38 Sample E CIGS / Mo / SS量測P-N示意圖 90
圖4-39 Sample F CIGS / Mo / SS量測P-N示意圖 91
圖4-40 Sample G CIGS / Mo / SS量測P-N示意圖 91
圖4-41 Sample H CIGS / Mo / SS量測P-N示意圖 92
圖4-42 ZnS / glass量測P-N示意圖 92
圖4-43 AZO / glass (ALD)量測P-N示意圖 93
圖4-44 AZO / glass (Sputter)量測P-N示意圖 93
圖4-45 鋁金屬電極外觀 94
圖4-46 不同堆疊之日光模擬系統檢測 95


















表目錄
表3-1　MO薄膜沈積於不鏽鋼基材之參數 51
表3-2　MO濺鍍於不銹鋼箔上之分析 53
表3-3　CIG前驅物薄膜濺鍍於MO/SS之參數 53
表3-4　前驅物之成份分析表 61
表3-5　硒化實驗參數 63
表4-1 CIG硒化後之成份分析 69
表4-2 不同堆疊之CIGS薄膜表面粗糙度 76
表4-3 不同堆疊之 CIGS( Smaple A、B、C、D ) 之 ( 112 ) 晶體結構關係 79
表4-4 不同堆疊之 CIGS( Smaple E、F、G、H ) 之 ( 112 ) 晶體結構關係 80
表4-5 ZnS薄膜沈積之參數 81
表4-6 濺鍍AZO薄膜沈積參數 85
表4-7 氧化鋅摻鋁薄膜沈積於Glass上之參數 85
表4-8 氧化鋅摻鋁薄膜沈積於Glass上之光穿透率 88
表4-9 正電極鋁金屬鍍製參數 94

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