臺灣博碩士論文加值系統

熱燈絲化學氣相沉積技術在沉積非晶，微晶及多晶矽薄膜於太陽電池的應用是極具潛力的一種技術。以熱燈絲化學氣相沉積矽薄膜比較於電漿輔助化學氣相沉積主要的優點為：(1) 無電漿轟擊，(2) 較高沉積速率，(3) 較低設備成本以及(4) 較高的氣體使用率，但可能遇到基板溫度控制不易及燈絲老化的問題。本論文主要探討非晶、微晶及多晶矽薄膜的沉積技術，特性分析及其應用。我們研究了氫稀釋比例、基板溫度及燈絲溫度等參數在沉積矽薄膜製程中的作用，同時我們也對不同參數製備之矽薄膜微結構進行研究探討。結果顯示矽薄膜的結晶率會隨著氫氣稀釋比例，基板溫度以及燈絲溫度的增加而增加，矽膜之含氫量隨著氫氣稀釋比例和基板溫度增加而減少但隨著燈絲溫度增加而增加。
本研究對於以熱燈絲化學氣相沉積技術沉積多晶矽薄膜之成長機制做深入研究，探討影響成長機制的參數以得到矽薄膜的特性最佳化。適度的調變參數下我們可以得到由完全非晶到93 %高結晶率的矽膜微結構特性，我們也觀察在非晶及多晶的轉變過程中氫氣稀釋比例和基板溫度的影響。
本論文同時探討以熱燈絲化學氣相沉積分別通入B2H6 或 PH3 摻雜氣體沉積p型及n型微晶矽薄膜，無論p型及n型微晶矽薄膜都可以利用現行本質矽薄膜沉積參數得到，使用1 %摻雜比例沉積n型微晶矽薄膜可以得到在太陽電池應用中可接受的電氣特性(σd = 0.292 Ω-1cm-1 and EA = 0.036 eV)。此外，使用1 %摻雜比例沉積p型微晶矽薄膜也可以得到接近0.15 Ω-1cm-1低的暗電導。最後我們利用熱燈絲化學氣相沉積技術沉積寬能隙及低活化能的p型及n型微晶矽薄膜實現高效率的異質接面矽太陽電池。
以上述之矽膜材料特性應用於p型單晶矽基板之異質接面太陽電池，我們初步研究了幾種不同的元件結構及特性。適度的氫氣處理及使用緩衝層可改善n層與單晶的界面，我們探討氫氣處理時間及n層厚度對於太陽電池性能的影響。比較對於基板不同的粗化結構光粹取效果的模擬與實驗結果，及不同粗化基板之異質接面矽太陽電池的效能。在氫氣處理時間及n層厚度等參數最佳化後，我們實現了短路電流為34.6 mA/cm2、開路電壓為 0.615 V、填充因子為 0.71及 效率為15.2 %之單面異質接面太陽電池元件。同時我們也完成了短路電流為34.8 mA/cm2、開路電壓為 0.645 V、填充因子為 0.73及效率為16.4 %之雙面異質接面太陽電池元件。
我們最後利用Pc1D軟體對異質接面太陽電池元件進行模擬，我們介紹太陽電池目前較常使用的模擬軟體並討論它們的發展及限制，接著提出模擬的結果。透過模組及數值模擬，針對元件串聯電阻、基板厚度、n層厚度、n層結晶率、i層厚度及i層結晶率對於太陽電池的影響做探討並且與實驗結果做比較。此目的在於瞭解元件參數的影響及元件最佳化設計，在最佳化太陽電池設計後之模擬結果，我們得到短路電流為39.4 mA/cm2、開路電壓為 0.64 V、 填充因子為 0.83及效率為21 %之異質接面太陽電池元件。這些結果對未來以熱燈絲化學氣相沉積技術低溫製造高效率異質接面太陽電池具有正面激勵的效果。

Hot-Wire Chemical Vapor Deposition (Hot-Wire CVD) is a promising technique for deposition of amorphous, microcrystalline and polycrystalline silicon thin films for photovoltaic applications. The main advantages of Hot-Wire CVD over PE-CVD, which is currently the most widespread applied technique to deposit thin silicon films in industry, are (1) absence of ion bombardment, (2) high deposition rate, (3) low equipment cost and (4) high gas utilization. Possible issues in Hot-Wire CVD are the control of the substrate temperature and aging of the filaments. This thesis deals with the full spectrum of deposition, characterization and application of amorphous, microcrystalline and polycrystalline silicon thin films. We studied the role of the hydrogen dilution ratio (DH), the substrate temperature (Ts) and the filament temperature (Tf) on the film parameters. Microstructures of the Si films with different deposition parameters have been investigated. It was found that an enhancement of crystallization with the increase of hydrogen dilution ratio, substrate temperature and filament temperature. The hydrogen content (CH) in the film decreases with increase in hydrogen dilution ratio and substrate temperature, but CH increases with increase in filament temperature.
A growth mechanism diagnosis for polycrystalline silicon deposition using Hot-Wire CVD is explored in this study. The role of the different parameters involved in the growth mechanism (filament temperature, substrate temperature and hydrogen dilution) was analyzed to optimize the properties of the deposited material. A wide range of microstructure features ranging from purely amorphous to highly crystalline (Xc > 0.93) was achieved after suitably tuning the deposition parameters. High Tf, Ts and/or DH allowed the deposition of highly crystalline material. Furthermore, an abrupt transition from a-Si to poly-Si was observed, especially when the influence of either DH or Ts were analyzed.
The ability to deposit both p- and n-type uc-Si doped layers by means of Hot-Wire CVD after the addition of B2H6 and PH3 respectively was evaluated. Both n-type and p-type materials were obtained in a relatively straightforward manner, as similar conditions to those leading to our state-of-the-art intrinsic silicon films could be employed. For n-type uc-Si films, the doping ratio (Sd) of 1 % was used leading to acceptable electrical properties (σd = 0.292 Ω-1cm-1 and EA = 0.036 eV), which allowed the incorporation of this material in photovoltaic devices. In addition, the deposition of p-type uc-Si material proved low σd (~ 0.15 Ω-1cm-1) was obtained when typical doping ratios at 1 % were employed. Finally, we achieved a high efficiency of heterojunction solar cell due to the high optical band gap and low activation energy of n-type and p-type uc-Si prepared by Hot-Wire CVD.
The above-mentioned results concerning material properties were applied in the deposition of our first p-type c-Si based heterojunction silicon solar cells grown by Hot-Wire CVD. These preliminary results concerned the analysis of several structures involving different device designs. The proper hydrogen pretreatment and buffer layer used in this work improves of n-layer/c-Si interface. The influences of hydrogen pre-treatment time and n-layer thickness on solar cell performance are studied. We investigated the light trapping effect of a silicon wafer with various pyramidal texture structures by simulation and experimental in this study. Ray-trace simulation in HJ silicon solar cells with various pyramidal texture structures was performed. After optimizing the deposition parameters of n-layer and the H2 pretreatment of solar cell, the single-side HJ solar cell with Jsc = 34.6 mA/cm2, Voc = 0.615 V, FF = 0.71, and efficiency of 15.1 % have been achieved. The double-side HJ solar cell with Jsc = 34.8 mA/cm2, Voc = 0.645 V, FF = 0.73, and efficiency of 16.4 % have been fabricated with optimum textured silicon substrate.
The behavior of our HJ solar cells was simulated using a Pc1D simulation program. We present a selection of currently available numerical simulation tools for heterojunction silicon solar cells, and discuss their possibilities and limitations. Afterwards, some results obtained with numerical simulation will be presented. By means of modeling and numerical computer simulation, the influence of series resistance of device, substrate thickness, n-layer emitter thickness, n-layer crystallinity, i-layer thickness and i-layer crystallinity on the solar cell performance (efficiency, open-circuit voltage, short-circuit current, fill factor and internal quantum efficiency) is investigated and compared with experimental results for p-type wafer material. It is the aim of this work to improve the understanding of this device and to derive arguments for design optimization. To evaluate device properties a numerical analysis of the experimental results have been proposed and discussed. After optimizing all the simulated parameters of solar cell, the best results with Jsc = 39.4 mA/cm2, Voc = 0.64 V, FF = 83 % and efficiency = 21 % has been achieved. These are very encouraging results for future fabrication of high efficiency heterojunction solar cells at low temperature by Hot-Wire CVD.

Abstract (in Chinese)...................................i
Abstract................................................iii
Contents................................................vi
List of tables..........................................x
List of figures.........................................xii
1. INTRODUCTION.........................................1
1.1 Solar energy........................................1
1.2 Why Si thin films...................................2
1.3 Amorphous, microcrystalline and polycrystalline silicon films...........................................4
1.4 Chemical Vapor Deposition (CVD).....................7
1.5 Plasma-Enhanced Chemical Vapor Deposition (PECVD)...8
1.6 Hot-Wire Chemical Vapor Deposition (Hot-Wire CVD)...9
1.7 What is the difference between Hot-Wire CVD and PECVD? ...............................................12
1.8 Major photovoltaic devices..........................15
1.9 Heterojunction silicon solar cell...................18
1.10 Aim of this work...................................20
1.11 Outline of this thesis.............................21
2. EXPERIMENTAL TECHNIQUES..............................24
2.1 Hot-Wire Chemical Vapor Deposition system...........24
2.2 Material characterization techniques................31
2.2.1 Optical measurement...............................31
2.2.2 Electrical measurement............................32
2.2.3 Raman spectroscopy................................34
2.2.4 X-ray diffraction (XRD)...........................36
2.2.5 Fourier-Transform Infrared Spectroscopy (FTIR)....37
2.2.6 Scanning Electron Microscopy (SEM)................39
2.2.7 Transmission Electron Microscopy (TEM)............40
2.2.8 Electron Paramagnetic Resonance (EPR).............40
2.2.9 Second ion mass spectroscopy (SIMS)...............43
2.2.10 Hall Effect measurement..........................44
2.3 Solar cell characterization.........................47
2.3.1 Current-voltage measurement.......................47
2.3.2 Quantum efficiency measurement....................49
3. DEPOSITION PROCESSES IN HOT-WIRE CVD.................51
3.1 Introduction........................................51
3.2 Deposition silicon films by Hot-Wire CVD............51
3.3 Gas dynamics in Hot-Wire CVD........................52
3.4 Reaction on catalyzer surface.......................52
3.5 Identification of radical species in gas phase......54
3.6 Film growth mechanism...............................55
4. HOT-WIRE DEPOSITED INTRENSIC SILICON FILMS...........57
4.1 Introduction........................................57
4.2 Silicon films deposited using W as filament.........59
4.2.1 Historical overview...............................59
4.2.2 Influence of the filament temperature.............60
4.2.2.1 Structure.......................................60
4.2.2.2 Optical properties..............................67
4.2.2.3 Electrical properties...........................68
4.2.3 Influence of the substrate temperature............69
4.2.3.1 Structure.......................................69
4.2.3.2 Optical properties..............................74
4.2.3.3 Electrical properties ..........................75
4.2.4 Influence of the hydrogen dilution................76
4.2.4.1 Structure.......................................76
4.2.4.2 Optical properties..............................82
4.2.4.3 Electrical properties...........................84
4.3 EPR and SIMS results of silicon films...............87
4.3.1 Defect density of silicon films determined by EPR measurement.............................................87
4.3.2 Contamination of silicon films determined by SIMS measurement.............................................90
4.4 Film growth mechanism in our research...............93
4.5 Summary............................................102
5. HOT-WIRE DEPOSITED P- AND N-TYPE SILICON FILMS......104
5.1 Introduction.......................................104
5.2 Experimental.......................................105
5.3 Electrical and optical properties..................106
5.4 Summary............................................111
6. HETEROJUNCTION SILICON SOLAR CELLS..................112
6.1 Introduction.......................................112
6.2 Experimental.......................................114
6.2.1 Substrate etching................................114
6.2.2 Texturing structure simulation...................114
6.2.3 Heterojunction silicon solar cell deposition.....116
6.2.4 ITO deposition...................................118
6.2.5 HJ solar cell characterization...................119
6.3 Results and discussion.............................119
6.3.1 Substrate texturing experimental and simulation..119
6.3.2 ITO properties...................................128
6.3.3 Heterojunction silicon solar cell results........133
6.3.3.1 Effect of hydrogen pretreatment................133
6.3.3.2 Effect of n-layer thickness....................136
6.3.3.3 Best results...................................139
6.4 Summary............................................143
7. SIMULATION OF HETEROJUNCTION SILICON SOLAR CELLS....144
7.1 Introduction.......................................144
7.2 Simulation.........................................146
7.2.1 Modeling.........................................146
7.2.2 Input parameters.................................148
7.3 Simulation results and discussion..................150
7.3.1 Effect of series resistance of device............150
7.3.2 Effect of substrate thickness....................154
7.3.3 Effect of n-layer thickness......................157
7.3.4 Effect of n-layer crystallinity..................161
7.3.5 Effect of i-layer thickness......................165
7.3.6 Effect of i-layer crystallinity..................169
7.3.7 Optimization of simulation results...............173
7.4 Summary............................................176
8. CONCLUSIONS AND FUTURE WORK.........................178
8.1 Conclusion.........................................178
8.2 Future work........................................180
References.............................................181
List of publications...................................201

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