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研究生： 陳家庠
Chen, Chia-Hsiang
論文名稱： 四元靶材濺鍍方式製備銅銦鎵硒太陽能電池
One-step sputtering process for CIGS solar cells application from a single quaternary target
指導教授： 賴志煌
Lai, Chih-Huang
口試委員: 曾百亨
Tseng, Bae-Heng
張正陽
Chang, Jenq -Yang
蔡松雨
Tsai, Song-Yeu
闕郁倫
Chueh, Yu-lun
賴志煌
Lai, Chih-Huang
學位類別： 博士
Doctor
系所名稱： 工學院 - 材料科學工程學系
Materials Science and Engineering
論文出版年： 2012
畢業學年度： 100
語文別： 英文
論文頁數： 191
中文關鍵詞： 薄膜太陽能電池 、銅銦鎵硒 、四元靶 、一段式 、濺鍍
外文關鍵詞： thin film solar cells, CIGS, quaternary target, one-step, sputter
相關次數： 點閱：1  下載：0 
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    • 近年來再生能源的議題持續發酵，太陽能便是其中一種深具潛力的選擇，許多類型的太陽能電池，包括單多介面砷化鎵、單多晶矽太陽能電池以及其他正在興起的技術已經被廣泛的研究，以期能取帶現有的發電技術。本論文主要的研究為銅銦鎵硒薄膜技術的開發，我們成功開發出簡單的一段式濺鍍銅銦鎵硒薄膜之製備方法並研究以此方式製備的薄膜及元件特性。
    在第四章的部分，我們的結果證明一段式濺鍍應用於製備銅銦鎵硒薄膜的可行性，藉由單一銅銦鎵硒四元靶材搭配脈衝直流濺鍍鍍方式在五百度的基版溫度下，即便沒有額外的硒供應，我們仍可製備出具有黃銅礦結構的銅銦鎵硒薄膜。而由此方式製備的銅銦鎵硒薄膜不同於傳統蒸鍍方式製備之特性，為具有（112）優選方向的柱狀晶結構，此外我們也針對此方式製備之薄膜及元件特性作進一步的探討與分析。在此章節，利用接近計量比的銅銦鎵硒靶材製備之元件，其最高效率可達到8.22 %。
    在第五章的部分，我們探討靶材成分對於銅銦鎵硒薄膜及元件的影響。藉由控制靶材成分，我們可以調變薄膜的組成從富銅相變至缺銅相，而富銅相銅銦鎵硒薄膜常見的銅硒二次相也可經由此方式有效降低，因此即便沒有氫化鉀處理的薄膜仍可得到極佳的元件表現，使用稍微缺銅且富硒的銅銦鎵硒四元靶材，我們得到最高效率達10.14 %之元件。此外我們也在銅銦鎵硒薄膜上開發出非破壞性的成分分析技術，藉由歐傑電子顯微鏡及場發式電子微探針技術，可以分析表面及內部成分之分布，我們發現造成富銅的銅銦鎵硒元件在長波長範圍的光電流響應較低的原因，應該跟不均勻的硒分布有關。
    在第六章的部分，我們探討如何藉由光學及電性的觀點改善元件之表現，包括鈉的摻雜以及奈米結構的導入。濺鍍氟化鈉製程目前的文獻中尚無報導，在本論文我們已成功將其與一段式濺鍍銅銦鎵硒薄膜製程整合，並觀察到明顯元件表現之提升，最高效率可達10.41 %。此外我們也開發出不需模版的方式製備銅銦鎵硒奈米針尖陣列，此奈米結構可以有效提升光捕獲效率並提升光電流之收集。

    Recently, solar energy has drawn much attention due to the development of renewable energy. Various solar cells have been widely studied for the application of solar energy to replace the conventional power for terrestrial application, including single/multi junction GaAs, crystalline Si cells (single/ multi crystalline), thin film technologies (CIGS, CdTe, amorphous-Si), and other emerging technologies. In this dissertation, the main research focus is on CIGS thin film technology. We have developed a simplified fabrication process and investigated the characteristics of CIGS solar cells prepared by the one-step sputtering process.
    In the first topic of this dissertation, we demonstrated the feasibility of one-step sputtering process for the fabrication of CIGS absorbers. By using pulse DC sputtering from a single quaternary CIGS target, the chalcopyrite structure is spontaneously developed on the substrate at 500 oC even without extra Se supply. The obtained CIGS absorber layer possesses unique columnar grains with (112) preferred orientation, which is quite different from those prepared by co-evaporation process. In addition, the characterization of one-step sputtered CIGS films and devices were also addressed. The best efficiency of 8.22 % was achieved at the area of 0.4 cm2 with open circuit voltage (Voc) of 505 mV, short circuit current density (Jsc) of 24.76 mA/cm2 and the fill factor (FF) of 0.66 by using a nearly stoichiometric CIGS target.
    The second topic of this dissertation focuses on the target composition effect on the CIGS films and devices. By tuning the composition of CIGS targets, we modified the film composition from Cu-rich to slight Cu-poor. In addition, the Cu2-xSe second phase was suppressed by using a modified CIGS target. Even no KCN treatment is required to obtain device quality CIGS films. The best device efficiency of 10.14 % was achieved at the area of 0.4 cm2 with open circuit voltage (Voc) of 505 mV, short circuit current density (Jsc) of 32.3 mA/cm2 and the fill factor (FF) of 0.63 by using a modified CIGS target. Furthermore, a non-destructive compositional mapping is demonstrated for the investigation of compositional distribution on the top surface and at deep level of CIGS films by using surface sensitive Auger electron spectroscopy (AES) and bulk sensitive field emission micro-analyzer (FE-EPMA). We found the inhomogeneous distribution of Se in the Cu-rich CIGS films may be related to the low photocurrent response in the long wavelength region. .
    The third topic in this dissertation focuses on the improvement of device performance. Na incorporation and nanostructure were introduced to modify the electrical and optical behaviors of CIGS solar cells. Sputtered NaF was first reported in this dissertation which could be integrated with our one-step sputtering process of CIGS absorbers. Better device efficiency of 10.41 % was observed while the NaF was added. Furthermore, we also developed a template-free technique to create nanotip arrays on the surface CIGS absorbers to enhance light harvesting, which could improve the collection of photocurrent.

    Abstract (in English) I Abstract (in Chinese) III Acknowledgements (in Chinese) V Table of contents VI List of figures X List of tables XIX Chapter 1 Introduction 2 1.1 Motivation 3 1.2 Dissertation Outline 9 Chapter 2 Literature Review 12 2.1 General introduction of solar cells 12 2.1.1 Current voltage characteristics 14 2.1.2 Materials selection of absorber layers 16 2.2 CIGS solar cells 18 2.2.1 Substrate 19 2.2.2 Mo back contact 21 2.2.3 CIGS absorber 23 2.2.5 Window layer 34 2.3 Fabrication process of CIGS absorbers 36 2.3.1 Evaporation 36 2.3.2 Selenization process 38 2.3.3 Sputtering process 41 2.4 Sodium incorporation 42 2.4.1 Na distribution within CIGS 44 2.4.2 Na effect on compositional properties 46 2.4.3 Na effect on structural properties 47 2.4.4 Na effect on electrical properties 49 Chapter 3 Experimental Techniques 52 3.1 Sample Fabrication 53 3.1.1 Magnetron Sputtering System 53 3.1.2 Annealing system 54 3.2 Structural Characterization 54 3.2.1 X-ray Diffraction 54 3.2.2 Scanning electron microscope (SEM) 55 3.2.3 Transmission Electron Microscope (TEM) 55 3.2.4 Atomic Force Microscope (AFM) 56 3.3 Optical characterization 57 3.3.1 UV-VIS-NIR spectrometer 57 3.3.2 Raman spectroscopy 58 3.3.3 Photoluminescence (PL) and time-resolved PL (TR-PL) spectroscopy 58 3.4 Compositional characterization 59 3.4.1 X-ray photoelectron spectroscopy(XPS) 59 3.4.2 Auger electron spectroscopy (AES) 60 3.4.3 Field emission electron probe micro-analyzer (FE-EPMA) 62 3.5 Device characterization 63 3.5.1 Current-voltage characterization 63 3.5.2 Quantum efficiency response (EQE) 63 3.5.3 Capacitance measurement (C-V) 64 Chapter 4 Characterization of CIGS films prepared by one-step sputtering process 68 4.1 Purpose of this study 68 4.2 Experiments 69 4.3 Results and discussion 71 4.3.1 Characteristics of CIGS target 71 4.3.2 Compositional properties of CIGS films 74 4.3.3 Structural properties of CIGS films 77 4.3.4 Optical properties of CIGS films 84 4.3.5 Microstructure and grain feature 92 4.3.6 Chemical structure of CIGS films 95 4.3.7 Electrical properties 99 4.4 Conclusion 105 Chapter 5 Target composition effect on the CIGS solar cells prepared by one-step sputtering process 108 5.1 Purpose of this study 108 5.2 Experiments 109 5.3 Results and discussion 112 5.3.1 Target composition effect on the film and device properties 112 5.3.2 Degradation mechanism of I-V behavior due to target composition effect 120 5.4 Conclusion 133 Chapter 6 The effects of post- and pre-treatment on CIGS device performance 136 6.1 Purpose of this study 136 6.2 Experiments 137 6.3 Discussion and results 139 6.3.1 Na incorporation 139 6.3.2 Nano structure for the application of CIGS solar cells 149 6.4 Conclusion 158 Chapter 7 Conclusions 162 Reference 166 Curriculum Vitae 186

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