光浸潤效應分析於化學水浴法氧化、硫化鋅薄膜緩衝層在銅銦鎵硒硫太陽能電池之研究

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研究生：	曹翔崴 Tsao, Hsiang-Wei
論文名稱：	光浸潤效應分析於化學水浴法氧化、硫化鋅薄膜緩衝層在銅銦鎵硒硫太陽能電池之研究 Investigation of Light Soaking Effect on Chemical Bath Deposited Zn(O,S) Buffer Layer-based Cu(In,Ga)(S,Se)2 Thin Film Solar Cells
指導教授：	闕郁倫 Chueh, Yu-Lun
口試委員:	張培俊 Chung, Pai-Chun 何頌賢 Ho, Johnny C.
學位類別：	碩士 Master
系所名稱：	工學院 - 材料科學工程學系 Materials Science and Engineering
論文出版年：	2018
畢業學年度：	107
語文別：	英文
論文頁數：	71
中文關鍵詞：	薄膜太陽能電池、化學水浴法、光浸潤效應、銅銦鎵硒硫、氧化、硫化鋅薄膜緩衝層
外文關鍵詞：	Light Soaking Effect, Chemical Bath Deposition, Thin Film Solar Cells, Cu(In,Ga)(S,Se)2, Zn(O,S) Buffer layer
相關次數：	點閱：162 下載：0
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對於高效能與可撓式薄膜光伏模組來說，銅銦鎵硒硫太陽能電池是具有發展前景的。無鎘緩衝層的應用是希望減少有毒元素的用量，硫化鋅與氧化鋅類的薄膜緩衝層在短波長(400-500奈米)吸收率較高，成為主流的替代緩衝層，而此種薄膜。然而，利用水浴法製程的硫化鋅薄膜緩衝層，必定含有氫氧化鋅，它會降低元件效能，只能通過長時間的光浸潤或光熱浸潤的手法來回復元件效能，這會拉長製造過程時程，並在使用產品時造成極大的不便。
為了克服這個問題，我們製造了銅銦鎵硒硫太陽能電池元件，其中利用化學水浴法（CBD）沉積出硫化鋅緩衝層，使用不同的水浴參數和後退火處理來比較。銅銦鎵硒硫太陽能電池的功率轉換效率和填充因子顯示出對氧化鋅薄膜緩衝層參數的相關性。當氧化鋅沉積在銅銦鎵硒硫薄膜上時，氫氧化鋅和氧化鋅也同時成長在此。由於氫氧化鋅的帶隙較低，能帶圖偏移使效率降低。經過光浸潤後，銅銦鎵硒硫太陽能電池的效率得到了改善。我們優化參數，減少光浸泡持續時間以達到功率轉換效率的飽和。也研究了在光浸潤下，隨時間的電性變化，並執行在光浸潤前後的SEM、TEM、XPS和EDX分析。

Cu(In,Ga)(S,Se)2(CIGSSe) based solar cells are promising candidates for high efficiency flexible thin film photovoltaic modules. To reduce the usage of toxic elements, it is desirable to apply cadmium-free buffer layer deposition process. Zn(O,S) based thin films have become the mainstream alternative buffer layer due to its low absorption in short wavelength region (400-500 nm). However, with chemical bath deposition (CBD)-ZnS buffer layer, it must have Zn(OH)2. The presence of Zn(OH)2 deteriorates the device performance and can only be recovered though time-consuming light or heat-light soaking procedures which slows down the manufacturing process and causes great inconvenience while using the products.
To overcome this obstacle, we fabricated CIGSSe solar cells with a CBD-ZnS buffer layer grown with varying aqueous solution recipe and post annealing treatments. The power conversion efficiency and the fill factor of the CIGSSe solar cells reveal a dependence on the deposition of CBD-ZnS films. When ZnS deposit on CIGSSe film, hydroxide and oxide species also deposit on it. Because of the lower band gap of Zn(OH)2, the resulting band diagram offsets deteriorates the efficiency. After the light soaking process, the performance of the CIGSSe solar cell was improved. We optimized the parameters in order to reduce the light soaking duration to reach the saturation of power conversion efficiency. We also measured the electrical properties of CIGSSe solar cells during light soaking process. To investigated the mechanism of the light soaking process, we took the SEM, TEM, XPS and EDX analysis before and after light soaking.

摘要    1
ABSTRACT    2
致謝    3
CONTENTS    4
LIST OF FIGURES    7
LIST OF TABLES    10
Chapter 1    Introduction    11
1.1.    Preface    11
1.2.    Different types of solar cell    13
1.2.1.    Silicon based solar cell    14
1.2.2.    Semiconductor compounds    15
1.2.3.    Emerging or novel materials    16
Chapter 2    Literature review and theoretical framework    18
2.1.    Basic principle and characteristic of solar cells    18
2.1.1.    Solar spectrum    18
2.1.2.    Basic principle of solar cell    21
2.2.    CIGS solar cell introduction    27
2.2.1.    CIGS introduction and development potential    27
2.2.2.    CIGS device structure    28
2.3.    Buffer layer of CIGS solar cells    31
2.3.1.    Types of buffer layer    31
2.3.2.    ZnS    32
2.3.3.    CBD-ZnS process    32
2.4.    Post treatments    34
2.4.1.    Ammonia solution etching    34
2.4.2.    Air Annealing    35
2.5.    Light soaking    36
2.6.    Motivation    38
Chapter 3    Experiment and Analysis    39
3.1.    Fabrication instrument    39
3.1.1.    Thermostatic bath    39
3.1.2.    Chemical    39
3.2.    Experimental procedure    40
3.2.1.    CBD-ZnS    40
3.2.2.    ZnO/ITO window layer and Al electrode    41
3.2.3.    Device measurement and light soaking    41
3.3.    Analysis instrument    42
3.3.1.    Solar cell simulator system    42
3.3.2.    UV -Visible Spectroscope    44
3.3.3.    Transmission electron microscope, TEM    45
3.3.4.    Scanning electron microscope, SEM    46
3.3.5.    Electron spectroscopy for chemical analysis    47
3.3.6.    Energy dispersive spectrometers, EDS    48
3.3.7.    Photoluminescence system, PL    49
3.3.8.    IPCE (Incident photon to current efficiency) / EQE (external quantum efficiency) System    51
Chapter 4    Results and Discussion    52
4.1.    Cleaning of CIGSSe surface    52
4.2.    Air annealing optimized    53
4.3.    CBD-ZnS    55
4.4.    Device performance and light soaking    56
4.5.    EQE analysis    58
4.6.    C-V measurement    59
4.7.    TEM-EDX analysis of the CIGSSe/ZnS interface    61
4.8.    XPS analysis    62
4.9.    Reversible characteristics of the light soaking effect    65
Chapter 5    Conclusions    67
Chapter 6    Future Perspective    68
Chapter 7    References    69

LIST OF FIGURES
Figure 1 1 World total installed capacity    12
Figure 1 2  Different types of solar cell[1]    13
Figure 1 3 Material absorption coefficient and photon energy diagram[2]    14
Figure 1 4 CIGS absorption layer structure (a) Zincblende (b) Chalcopyrite    16
Figure 2 1 Solar spectrum at the top of the atmosphere and at sea level[3]    20
Figure 2 2 The definition of AM parameter[4]    20
Figure 2 3 Solar cell structure: p-n junction diode    22
Figure 2 4 Solar cell equivalent circuit    24
Figure 2 5 CIGS solar cell I-V curve    26
Figure 2 6 Best research-cell efficiencies[5]    28
Figure 2 7 CIGS device structure    30
Figure 2 8 (a) Hexagonal (Wurtzite) crystal structure; (b) Cubic (zinc blende) structure    32
Figure 2 9 SEM photograph of ZnS(O,OH) buffer layer deposited on a CIGS thin film with (right) and without (left) ammonia rinsing.    34
Figure 2 10 I-V characteristics of CBD-ZnS/CIGS solar cells (a) without and (b) with ammonia rinsing    35
Figure 2 11 I-V characteristics of the ZnS/CIGS solar cells (a) without and (b) with air annealing at 200℃ for 10 mins    36
Figure 2 12 Zn(S,O) band gap change with composition by ALD[30]    37
Figure 2 13 Device efficiency changes with H2S/(H2O+H2S)[30]    38
Figure 3 1 CBD-ZnS process steps    40
Figure 3 2 NH4OH etching and air annealing process    41
Figure 3 3 Light soaking conditions    42
Figure 3 4 The spectrum of the AM 0 and AM 1.5 at 6000k    43
Figure 3 5 Solar cell simulator system    43
Figure 3 6 UV -Visible Spectroscope (Hitachi U-4100)    44
Figure 3 7 Japan JEOL JEM-F200 HRTEM    45
Figure 3 8 ESCA of ULVAC-PHI PHI 5000 Versaprobe II    48
Figure 3 9 EDS element analysis    49
Figure 3 10 Photoluminescence principle diagram    50
Figure 3 11 Photoluminescence system diagram    50
Figure 4 1 Etching process by HCl and NH4OH solution    52
Figure 4 2 SEM/EDX and EDX spectrum    53
Figure 4 3 Heating curve of air annealing    54
Figure 4 4 UV-Visible spectrum with different reaction time    55
Figure 4 5 (a) Top view and (b) cross section of SEM image    56
Figure 4 6 Electrical measurement of (a) Jsc, (b) Voc, (c) Fill factor and (d) Efficiency during light soaking    57
Figure 4 7 Static plot of measurement for (a) Jsc, (b) Voc, (c) Fill factor and (d) Efficiency before and after light soaking    58
Figure 4 8 EQE spectra of (a) 17 mins,(b) 20 mins and (c) 22 mins before and  after light soaking of different reaction time    59
Figure 4 9 C-V measurement for (a) t=17 mins (b) t=20 mins (c) t=22 mins before and after light soaking    60
Figure 4 10 TEM images and EDX data of (a) t=17 mins, (b) t=20 mins and (c) t=22 mins the ZnS/CIGSSe interface    61
Figure 4 11 TEM-EDX S/(S+O) ratio of (a) t=17 mins , (b) t=20 mins and (c) t=22 mins    62
Figure 4 12 XPS measurement of Zn2P bonding energy before and after light soaking    63
Figure 4 13 Peak fitting of Zn2P (a) before and (b) after light soaking    63
Figure 4 14 XPS profile (a) before and (b) after light soaking    64
Figure 4 15 S/(S+O) profile of t=22 mins before and after light soaking    65
Figure 4 16 Comparison of light soaking after 21 days for (a) t=17 mins, (b) t=20 mins and (c) t=22 mins    66

LIST OF TABLES
Table 1 1 Yearly Solar Fluxes & Human Energy Consumption    12
Table 4 1 Compositions of EDX analysis    53
Table 4 2 Temperature optimized of air annealing    54
Table 4 3 Time optimized of air annealing    54
Chapter 1

                                

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