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研究生:邱俊閎
研究生(外文):Chun-Hong Chiu
論文名稱:堆疊式形成二硒化銅銦薄膜的研究
論文名稱(外文):A study of CIS thin films prepared by SEL technique
指導教授:彭洞清
指導教授(外文):Dung-Ching Perng
學位類別:碩士
校院名稱:國立成功大學
系所名稱:微電子工程研究所碩博士班
學門:工程學門
學類:電資工程學類
論文種類:學術論文
畢業學年度:96
語文別:英文
論文頁數:62
中文關鍵詞:二硒化銅銦化學槽水域法元素堆疊
外文關鍵詞:SELCuInSe2(CIS)Chemical bath deposition(CBD)
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二硒化銅銦(CIS)化合物半導體在I-III-VI2 族太陽能電池中,佔很重要的角色,因為它有高的光電轉換效率、高可靠度以及低製程成本的優點。二硒化銅銦對光的吸收係數相當高 (~105 cm -1),只要大約2 μm厚的吸收層,就可吸收大部份的太陽光波段。在實驗室最常採用的製程方法是在有基板加熱下同步蒸鍍(co-evaporation)銅銦硒的製程,以及在硒化氫(H2Se)或硒(Se)氣體環境下,將銅銦前驅物(Cu-In presursor)高溫硒化 (selenization)。不過這兩種形成二硒化銅銦的製程都有毒性問題與對環境有害的問題。
本論文主要是利用一種沒有毒氣問題的方法沉積硒薄膜,再比較不同的元素堆疊(stack element layer, SEL)方式,選擇一種最好的堆疊結構(銦/硒/銅)與硒化時的溫度曲線(annealing temperature profile),將組成比例接近1:1:2的二硒化銅銦薄膜得到。沉積硒(selenium)薄膜是採用化學槽水域法(chemical bath deposition, CBD),沉積銅(copper)薄膜與銦(indium)薄膜是使用濺鍍法 (sputtering)。沉積硒薄膜採用化學槽水域的好處是它不必擔心毒氣外洩的問題,製程成比也相當的便宜。
為了將化學槽水域法所得到的硒薄膜應用到堆疊結構中,我們會得到一個理想的製程條件,來沉積足夠厚的硒薄膜,已使得硒化後硒元素的含量接近50at.%。應用到堆疊結構中後,將會比較各種不同的堆疊結構,找到一個最適合的堆疊方式,進行硒化。而硒化時的溫度曲線,也會找到最適合的溫度曲線來進行硒化,使得硒化後二硒化銅銦薄膜的厚度可達大約2 μm,銅元素、銦元素與硒元素的比例會接近1:1:2的組成比例(stoichiometry)。由於銅元素與銦元素(Cu/In)最理想的比例在0.7-1.0之間,所以我們將銅元素與銦元素的比例控制成0.77,進行物理特性的分析。由XRD分析可得到一很強的(112)結晶平面,由SEM分析可得到晶粒大小(grain sizes)大約2-2.5 μm。
I-III-VI2 solar cells such as CuInSe2 (CIS) compound semiconductor is a great candidate for large-area solar panels because of its high efficiency, reliable long-term performance and potential for low-cost production. The high absorption coefficient (~105 cm -1) can be obtained from a thin CIS layer. A 2 μm CIS film is sufficient to absorb the most useful part of the solar spectrum. The most widely accepted methods are co-evaporation of the elements on heated substrate and annealing of Cu-In precursors in H2Se or Se atmosphere. Both processes are extremely toxic to health and harmful to environment.

In my thesis, a new approach to form CIS absorber film is presented. Ternary semiconductor CIS thin films prepared by stack element layer (SEL) technique (i.e. In/Se/Cu, etc.) using sputtering for Cu/In and chemical bath deposition (CBD) technique for Se followed by a one-step selenization. The advantages of using CBD Se process is that it is a low-cost process and pollution free, i.e. it totally avoided usage of highly toxic H2Se or Se vapor.

The studies of growth CBD Se versus deposition time have been carried out. Thick enough CBD Se film and proper Cu/In thickness can fabricate 2 μm thick CIS film. Different stacking sequences to form CIS absorber were studied by comparing the reaction mechanisms. In/Se/Cu is the best stacking structure for preparing CIS absorber films. Using this structure, we have achieved a close 1:1:2 stoichiometicy ratio for Cu, In and Se,respectively. Thin film has a high XRD intensity on the CIS (112) plane. The total thickness of the CIS film was about 2μm and had grain sizes of 2 - 2.5 μm.
Chinese abstract
English abstract
Contents
Table Captions
Figure Captions
Chapter 1 Introduction
1.1 Brief History of photovoltaic (PV).……………………1
1.2 Why we need PV ………………………………………………3
1.3 How Solar Cells Work ………………………………………5
1.3.1 Air Mass and Solar Spectrum……………………………7
1.3.2 Solar Cell I-V Characteristics………………………10
1.3.3 Additional important parameters ……………………13

Chapter 2 Introduction to CIS&CIGS solar cells
2.1 The properties of Chalcopyrite-based materials ……18
2.2 Development of CIS&CIGS thin film solar cells ……23
2.3 Reaction mechanism of CIS formation……………………26
2.4 The compositional analysis ………………………………28

Chapter 3 Experimental Scheme
3.1 Purposes of this experiment………………………………29
3.2 Experiment procedures………………………………………30
3.3 Experiment equipments………………………………………33
3.3.1 Sputter system ……………………………………………33
3.3.2 Annealing system …………………………………………35
3.4 Analysis equipments…………………………………………37
3.4.1 X-ray diffraction (XRD) ………………………………37
3.4.2 Scanning Electron Microscope (SEM) …………………38
3.4.3 X-ray energy dispersive (EDS) ………………………40

Chapter 4 Results and Discussions
4.1 Se prepared by CBD technique ……………………………41
4.1.1 The CBD Se growth study…………………………………41
4.1.2 The compositional analysis ……………………………44
4.2 CIS film prepared by SEL technique ……………………48
4.3 The stoichiometry of the post annealed film using sequence In/Se/Cu…………………………………………………58

Chapter 5 Conclusions and Future works
5.1 Conclusion ……………………………………………………60
5.2 Future works …………………………………………………62
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