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本研究利用共蒸鍍法製備銅銦鎵金屬合金前驅物薄膜，再以退火
及 硒 化 的 方 式 ， 於 玻 璃 或 銦 錫 氧 化 物 （ ITO ） 基 材 上 製 備 出
Cu-In-Ga-Se四元化合物半導體薄膜，並探討不同銅銦鎵比例對於薄
膜結構、光學性質、光電化學反應性質以及導電型態的影響。
由 X 光繞射分析儀（XRD）分析結果可知，於不同銅銦鎵比例
下，皆可製備出具黃銅礦結構的 CuIn 1-x Ga x Se 2 （x = 0～1）薄膜，
而由能量分散式 X 光元素分析儀（EDAX）分析結果與光學量測結
果可得知，隨著薄膜中鎵含量的增加或銅含量的減少，薄膜的直接能
隙會從1.28 eV 上升至 1.50 eV。薄膜厚度約為 1.8~4 µm之間。在光
電流密度量測中，將薄膜置於 0.35M之Na 2 S及0.25M之K 2 SO 3 混合之
水溶液可得到最高光敏化效果0.24 mA/cm
2 。在薄膜電性量測方面，
可發現隨著薄膜中銅含量的減少，載子濃度會下降，電阻率會上升，
而導電型態皆為p-type。
以glass/Mo/CIGS/CdS/IZO/AZO/Ag為結構製備光電池之開環電
壓為0.238 V，短路電流為 0.134 mA/cm
2
，光電轉換效率η為 0.01 %，
FF 值為 0.220。

In this study, the Cu-In-Ga-Se (CIGS) semiconductor
thin films were deposited on glass substrates and
indium-tin-oxide (ITO) coated glass substrates using
selenization of co-evaporated Cu-In-Ga metal alloys . The
effect of the Cu/(In+Ga) and Ga /(In+Ga) molar ratio in
Cu-In-Ga metal alloys on the structural, optical and
electrical properties of CIGS thin film were investigated.
X-ray diffraction pattern of samples ( XRD ) revealed
that samples in this study were chalcopyrite CIGS phase.
Energy dispersive analysis of X-ray ( EDAX ) showed that
compositions of CuIn 1-x Ga x Se 2 thin film were the function
of the Cu-In-Ga molar ratio in metal alloys. The
thickness of samples were in the range of 1.8 ~ 4 µm. The
direct energy band gap of samples varied from 1.28~ 1.50
eV, depending on Cu/(In+Ga) and Ga/(In+Ga) molar ratios
in samples. Maximum photocurrent density of samples
reached to 0.24 mA/cm
2
in the solution containing S
2-

and SO 3
2-
ions. The carrier concentration of samples varied
from 2.86 × 10
18
~ 3.82 × 10
12
cm
-3
using Hall measurement.
The resistivity of samples decreased with an increase in
Cu/(In+Ga) molar ratio in samples. The conduction type of
CuIn 1-x Ga x Se 2 thin films are all p-type.
Glass/Mo/CIGS/CdS/IZO/AZO/Ag solar cell gaved V OC
of 0.238 V, J SC of 0.134 mA/cm
2
, FF of 0.220, and
conversion efficiency of 0.01 %.

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目錄
致謝 ................................................................................................................ iv
摘要 .................................................................................................................. v
Abstract .......................................................................................................... vi
目錄 .............................................................................................................. viii
圖目錄 ............................................................................................................ xi
表目錄 ........................................................................................................ xviii
第一章 緒論.................................................................................................... 1
1.1 前言 ..................................................................................................... 1
1.2 研究目的 ............................................................................................. 2
第二章 理論與文獻回顧 ............................................................................... 5
2.1 半導體性質 ......................................................................................... 5
2.1.1 半導體能帶理論 ....................................................................... 6
2.1.2 費米能階 ................................................................................... 7
2.1.3 直接能隙與間接能隙 .............................................................. 8
2.2 太陽能電池理論 ................................................................................. 8
2.2.1 光電效應 ................................................................................... 9
2.2.2 p-n 接面 .................................................................................. 10
2.2.3 光伏效應 ................................................................................. 11
ix

2.2.4 常見的太陽能電池材料 ......................................................... 11
2.3 CuIn 1-x Ga x Se 2 ( CIGS ) 材料簡介 ............................................... 13
2.4 製備方法 ........................................................................................... 14
2.4.1 化學水浴沈積法 ..................................................................... 14
2.4.2 噴霧熱解法 ............................................................................. 14
2.4.3 塗布法 ..................................................................................... 15
2.4.4 電沈積法 ................................................................................. 15
2.4.5 分子束磊晶 ............................................................................ 16
2.4.6 濺鍍法 ..................................................................................... 16
2.4.7 共蒸鍍法 ................................................................................. 17
第三章 實驗.................................................................................................. 25
3.1 實驗藥品 ........................................................................................... 25
3.2 實驗儀器與設備 ............................................................................... 26
3.2.1 薄膜製程設備 ......................................................................... 26
3.2.2 分析儀器與設備 ..................................................................... 27
3. 3 實驗流程 .......................................................................................... 28
3.3.1 基材清洗 ................................................................................ 28
3.3.2 銅、銦、鎵預成薄膜比例計算 ............................................ 28
3.3.2 銅、銦、鎵預成薄膜比例計算 ............................................ 29
x

3.3.3 預成薄膜製備步驟 ................................................................ 29
3.3.4 金屬預成薄膜熱處理 ............................................................. 31
3.3.5 薄膜硒化 ................................................................................. 31
3. 4 薄膜性質分析 .................................................................................. 32
第四章 結果與討論 ..................................................................................... 39
4.1 薄膜晶型結構分析........................................................................... 39
4.2 薄膜元素分析 ................................................................................... 41
4.3 薄膜表面型態分析........................................................................... 43
4.4 膜厚分析 ........................................................................................... 44
4.5 薄膜光學性質分析........................................................................... 44
4.6 薄膜電性量測 ................................................................................... 47
4.7 光電流密度量測 ............................................................................... 48
4.8 CuIn 1-x Ga x Se 2 太陽能電池............................................................... 49
第五章 結論與未來展望 ........................................................................... 93
參考文獻 ........................................................................................................ 95



xi

圖目錄
圖 1-1、1999～2007 年全球各國太陽能電池之裝置容量 ......................... 4
圖 2-1、導體、半導體、絕緣體等固體材料電導率(電阻率)範圍 ......... 20
圖 2-2、n 型半導體電子移動示意圖 ......................................................... 20
圖 2-3、p 型半導體電洞移動示意圖 ......................................................... 21
圖 2-4、分子軌域混成示意圖 .................................................................... 21
圖 2-5、費米能階（E F ）於 n 型和 p 型半導體中之位置 ........................ 22
圖 2-6、（a）直接能隙與（b）間接能隙 E-k 關係圖 ............................ 22
圖 2-7、p-n 接面之空間電荷區 .................................................................. 23
圖 2-8、2001 年各種太陽能電池材料之市場分佈率 ............................... 23
圖 2-9、黃銅礦結構 .................................................................................... 24
圖 2-10、共蒸鍍製程設備示意圖 .............................................................. 24
圖 3-1、熱蒸鍍機示意圖 ............................................................................ 33
圖 3-2、光電化學反應裝置圖 .................................................................... 34
圖 3-3、實驗流程圖 .................................................................................... 35
圖 4-1、銅銦鎵硒合金相圖 ........................................................................ 52
圖 4-2、溫度 150℃、225℃退火 30 分鐘，溫度 500℃、550℃硒化
30 分鐘之 XRD 圖 ........................................................................................ 52

xii

圖 4-3、溫度 250℃退火 30 分鐘，溫度 500℃、550℃硒化 30 分鐘之
XRD 圖 ......................................................................................................... 53
圖 4-4、溫度 250℃退火，溫度 550℃硒化不同時間之 XRD 圖 .......... 53
圖 4-5、溫度 150℃、250℃退火 30 分鐘，溫度 500℃、550℃硒化 60
分鐘之 XRD 圖 ........................................................................................... 54
圖 4-6、不同銅比例之 XRD 圖 ................................................................... 54
圖 4-7、不同鎵比例之 XRD 圖 ................................................................... 55
圖 4-8、不同銅理論比例對 EDAX 分析所得之銅比例作圖 .................. 55
圖 4-9、不同鎵理論比例對 EDAX 分析所得之鎵比例作圖 .................. 56
圖 4-10、Sample（C1）（Cu/In+Ga EDAX 比例為 1.01）之 SEM 表
面圖。 ............................................................................................................ 56
圖 4-11、Sample（C2）（Cu/In+Ga EDAX 比例為 0.96）之 SEM 表
面圖。 ............................................................................................................ 57
圖 4-12、Sample（C3）（Cu/In+Ga EDAX 比例為 0.75）之 SEM 表
面圖 ................................................................................................................ 57
圖 4-13、Sample（C4）（Cu/In+Ga EDAX 比例為 0.71）之 SEM 表
面圖 ................................................................................................................ 58
圖 4-14、Sample（C5）（Cu/In+Ga EDAX 比例為 0.58）之 SEM 表
面圖 ................................................................................................................ 58
xiii

圖 4-15、Sample（C6）（Cu/In+Ga EDAX 比例為 0.50）之 SEM 表
面圖 ................................................................................................................ 59
圖 4-16、Sample（C7）（Cu/In+Ga EDAX 比例為 0.48）之 SEM 表
面圖 ................................................................................................................ 59
圖 4-17、Sample（C1）（Cu/In+Ga EDAX 比例為 1.01）之 SEM 側
面圖 ................................................................................................................ 60
圖 4-18、Sample（C2）（Cu/In+Ga EDAX 比例為 0.96）之 SEM 側
面圖 ................................................................................................................ 60
圖 4-19、Sample（C3）（Cu/In+Ga EDAX 比例為 0.75）之 SEM 側
面圖 ................................................................................................................ 61
圖 4-20、Sample（C4）（Cu/In+Ga EDAX 比例為 0.71）之 SEM 側
面圖 ................................................................................................................ 61
圖 4-21、Sample（C5）（Cu/In+Ga EDAX 比例為 0.58）之 SEM 側
面圖 ................................................................................................................ 62
圖 4-22、Sample（C6）（Cu/In+Ga EDAX 比例為 0.50）之 SEM 側
面圖 ................................................................................................................ 62
圖 4-23、Sample（C7）（Cu/In+Ga EDAX 比例為 0.48）之 SEM 側
面圖 ................................................................................................................ 63

xiv

圖 4-24、Sample（G1）（Ga/In+Ga EDAX 比例為 0.43）之 SEM 表
面圖 ................................................................................................................ 63
圖 4-25、Sample（G2）（Ga/In+Ga EDAX 比例為 0.35）之 SEM 表
面圖 ................................................................................................................ 64
圖 4-26、Sample（G3）（Ga/In+Ga EDAX 比例為 0.30）之 SEM 表
面圖 ................................................................................................................ 64
圖 4-27、Sample（G4）（Ga/In+Ga EDAX 比例為 0.23）之 SEM 表
面圖 ................................................................................................................ 65
圖 4-28、Sample（G5）（Ga/In+Ga EDAX 比例為 0.19）之 SEM 表
面圖 ................................................................................................................ 65
圖 4-29、Sample（G1）（Ga/In+Ga EDAX 比例為 0.43）之 SEM 側
面圖 ................................................................................................................ 66
圖 4-30、Sample（G2）（Ga/In+Ga EDAX 比例為 0.35）之 SEM 側
面圖 ................................................................................................................ 66
圖 4-31、Sample（G3）（Ga/In+Ga EDAX 比例為 0.30）之 SEM 側
面圖 ................................................................................................................ 67
圖 4-32、Sample（G4）（Ga/In+Ga EDAX 比例為 0.23）之 SEM 側
面圖 ................................................................................................................ 67

xv

圖 4-33、Sample（G5）（Ga/In+Ga EDAX 比例為 0.19）之 SEM 側
面圖 ................................................................................................................ 68
圖 4-34、不同銅比例（Cu/In+Ga 理論比例 0.41~97）之 CuIn 1-x Ga x Se 2
薄膜穿透率圖譜 ........................................................................................... 68
圖 4-35、不同鎵比例（Ga/In+Ga 理論比例 0.23~54）之 CuIn 1-x Ga x Se 2
薄膜穿透率圖譜 ........................................................................................... 69
圖 4-36、不同銅比例（Cu/In+Ga 理論比例 0.41~97）之 CuIn 1-x Ga x Se 2
薄膜反射率圖譜 ........................................................................................... 69
圖 4-37、不同鎵比例（Ga/In+Ga 理論比例 0.23~54）之 CuIn 1-x Ga x Se 2
薄膜反射率圖譜 ........................................................................................... 70
圖 4-38、不同銅比例（Cu/In+Ga 理論比例 0.41~97）之 CuIn 1-x Ga x Se 2
薄膜 (αhν)
2
vs. hν 圖 .................................................................................... 70
圖 4-39、薄膜中 Cu/In+Ga 比例與能隙之關係圖 ................................... 71
圖 4-40、不同鎵比例（Gu/In+Ga 理論比例 0.23~54）之 CuIn 1-x Ga x Se 2
薄膜 (αhν)
2
vs. hν 圖 .................................................................................... 71
圖 4-41、薄膜中 Ga/In+Ga 比例與能隙之關係圖 ................................... 72
圖 4-42、CuIn 1-x Ga x Se 2 薄膜其 Cu/In+Ga 比例對載子濃度及電阻率作
圖 .................................................................................................................... 72

xvi

圖 4-43、CuIn 1-x Ga x Se 2 薄膜其 Ga/In+Ga 比例對載子濃度及電阻率
作圖 ................................................................................................................ 73
圖 4-44、Sample（C1）（Cu/In+Ga EDAX 比例為 1.01）)的光敏化
效應量測圖 .................................................................................................... 73
圖 4-45、Sample（C2）（Cu/In+Ga EDAX 比例為 0.96）)的光敏化
效應量測圖 .................................................................................................... 74
圖 4-46、Sample（C3）（Cu/In+Ga EDAX 比例為 0.75）的光敏化效
應量測圖 ........................................................................................................ 74
圖 4-47、Sample（C4）（Cu/In+Ga EDAX 比例為 0.71）的光敏化效
應量測圖 ........................................................................................................ 75
圖 4-48、Sample（C5）（Cu/In+Ga EDAX 比例為 1.01）)的光敏化
效應量測圖 .................................................................................................... 75
圖 4-49、Sample（C6）（Cu/In+Ga EDAX 比例為 0.50）的光敏化效
應量測圖 ........................................................................................................ 76
圖 4-50、Sample（C7）（Cu/In+Ga EDAX 比例為 0.48）的光敏化效
應量測圖 ........................................................................................................ 76
圖 4-51、Sample（G1）（Ga/In+Ga EDAX 比例為 0.43）的光敏化
效應量測圖 .................................................................................................... 77
圖 4-52、Sample（G2）（Ga/In+Ga EDAX 比例為 0.35）的光敏化
xvii

效應量測圖 .................................................................................................... 77
圖 4-53、Sample（G3）（Ga/In+Ga EDAX 比例為 0.30）的光敏化
效應量測圖 .................................................................................................... 78
圖 4-54、Sample（G4）（Ga/In+Ga EDAX 比例為 0.23）的光敏化
效應量測圖 .................................................................................................... 78
圖 4-55、Sample（G5）（Ga/In+Ga EDAX 比例為 0.19）的光敏化
效應量測圖 .................................................................................................... 79
圖 4-56 、 glass/Mo/CIGS/CdS(In 2 S 3 )/IZO/AZO/Ag 光 電 池 模 組 結
構圖 ................................................................................................................ 79
圖 4-57、glass/Mo/CIGS/CdS(In 2 S 3 )/IZO/AZO/Ag 太陽能電池模組裝
置圖 ................................................................................................................ 80
圖 4-58、glass/Mo/G2/ CdS /IZO/AZO/Ag 太陽能電池模組效率量測圖
........................................................................................................................ 80
圖 4-59、glass/Mo/G3/In 2 S 3 /IZO/AZO/Ag 太陽能電池模組效率量測
圖 .................................................................................................................... 81
圖 4-60、glass/Mo/G4/In 2 S 3 /IZO/AZO/Al/Ni 太陽能電池模組效率量
測圖 ................................................................................................................ 81
圖 4-61、glass/Mo/G5/In 2 S 3 /IZO/AZO/ Al/Ni 太陽能電池模組效率量
測圖 ................................................................................................................ 81
xviii

表目錄
表 3-1、改變不同退火及硒化溫度及時間參數表 .................................... 36
表 3-2、改變銅比例之共蒸鍍源銅銦鎵金屬質量參數表 ........................ 37
表 3-3、改變銦鎵比例之共蒸鍍源銅銦鎵金屬質量參數表 .................... 38
表 4-1、不同退火及硒化參數 XRD 晶相分析整理表 ............................. 82
表 4-2、不同銅比例下，退火前之銅銦鎵金屬薄膜元素分析表 ............ 83
表 4-3、不同銅比例下，硒化後之 CuIn 1-x Ga x Se 2 薄膜元素分析表 .... 84
表 4-4、不同鎵比例下，退火前之鎵成分元素分析表 ............................ 85
表 4-5、不同鎵比例下，硒化後之 CuIn 1-x Ga x Se 2 薄膜元素分析表 .... 86
表 4-6、不同銅比例之 CuIn 1-x Ga x Se 2 薄膜其厚度與直接能隙值 ...... 87
表 4-7、不同鎵比例之 CuIn 1-x Ga x Se 2 薄膜其厚度與直接能隙值 ...... 88
表 4-8、不同銅比例下之 CuIn 1-x Ga x Se 2 薄膜其霍爾量測數據表 ........ 89
表 4-9、不同鎵比例下之 CuIn 1-x Ga x Se 2 薄膜其霍爾量測數據表 ........ 90
表 4-10、不同銅比例之 CuIn 1-x Ga x Se 2 薄膜之光敏化效果 ................ 91
表 4-11、不同鎵比例之 CuIn 1-x Ga x Se 2 薄膜之光敏化效果 ................ 92

95

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