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研究生： 阮江南
Nguyen - Giang Nam
論文名稱： Development of ZnO:Ga Transparent Conducting Oxide Thin Films through Metalorganic Chemical Vapor Deposition using various Zn and Ga Source Materials
Development of ZnO:Ga Transparent Conducting Oxide Thin Films through Metalorganic Chemical Vapor Deposition using various Zn and Ga Source Materials
指導教授： 洪儒生
Lu-Sheng Hong
口試委員: 江志強
Jyh-Chiang Jiang
黃鶯聲
Ying-Sheng Huang
陳敏璋
Miin-Jang Chen
盧信冲
Hsin-Chun Lu
邱正杰
Jaychu
學位類別： 博士
Doctor
系所名稱： 工程學院 - 化學工程系
Department of Chemical Engineering
論文出版年： 2013
畢業學年度： 101
語文別： 英文
論文頁數： 75
中文關鍵詞： 透明導電氧化物 、氧化鋅 、有機金屬化學氣相沉積 、氧化鋅鎵 、三甲基鎵 、三乙基鎵
外文關鍵詞： TCO, ZnO, MOCVD, GZO, TMG
相關次數： 點閱：266  下載：4 
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  •  上一筆

    • The Ga doped-ZnO (GZO) thin film has been demonstrated to have low resistivity and high transparency in the visible spectral range and that is considered as one of the most promising transparent conducting oxide (TCO) for the next generation of transparent electrode materials. There is still much to be explored and understood about main factor that significantly affect to the properties as well as the cost of GZO film growth process before it can be commercially realized. Most notably, the influence of the type of source materials have surprisingly been received less attention, even though the type of sources actually play critically role not only the quality but also the cost of thin films. In this dissertation, we have developed of GZO TCO thin films through metalorganic chemical vapor deposition (MOCVD) using various Zn source materials. We also explored the methodology to increase the light diffuse transmittance through controlling the preferred orientation of polycrystalline GZO films by MOCVD technique using diethyl zinc (DEZn) as the Zn and trimethylgallium (TMG) as a Ga precursor.
    We prepared Ga-doped ZnO (GZO) films with qualified opto-electric properties through chemical vapor deposition of an inexpensive solution of DEZn in n-hexane (ca. 17 wt.%). The GZO films exhibited low resistivity (3.61  10–4 Ω cm) and high transmittance (85%) in the visible range. Interestingly, post-annealing treatment of the GZO films under N2 at 525 °C for just 10 min increased the number of carbon-interstitial oxygen defects (CZn+2Oi)〃, which played the role of acceptors and enhanced the film properties significantly. This approach potentially allows the fabrication of inexpensive transparent conducting oxides for use in solar cells.
    Moreover, we also explored the methodology to increase the light diffuse transmittance through controlling the preferred orientation of polycrystalline GZO films grown by the low-pressure chemical vapor deposition (LPCVD) technique. X-ray diffraction measurement indicated that major growth direction was (002) plane and secondary electron microscopy showed that column-like granule structure with planar surface was formed. By depositing a low temperature ZnO layer to serve as a template for high temperature GZO film growth, the main preferred orientation of the GZO films was manipulated to (110) plane and the film surface to the pyramid-like structure. Through this two-step growth, the light diffuse transmittance of the film with a GZO (800 nm)/ZnO (766 nm) combination exhibited 13% increase at 420 nm wavelength due to the preservation of the pyramidal surface morphology.

    The Ga doped-ZnO (GZO) thin film has been demonstrated to have low resistivity and high transparency in the visible spectral range and that is considered as one of the most promising transparent conducting oxide (TCO) for the next generation of transparent electrode materials. There is still much to be explored and understood about main factor that significantly affect to the properties as well as the cost of GZO film growth process before it can be commercially realized. Most notably, the influence of the type of source materials have surprisingly been received less attention, even though the type of sources actually play critically role not only the quality but also the cost of thin films. In this dissertation, we have developed of GZO TCO thin films through metalorganic chemical vapor deposition (MOCVD) using various Zn source materials. We also explored the methodology to increase the light diffuse transmittance through controlling the preferred orientation of polycrystalline GZO films by MOCVD technique using diethyl zinc (DEZn) as the Zn and trimethylgallium (TMG) as a Ga precursor.
    We prepared Ga-doped ZnO (GZO) films with qualified opto-electric properties through chemical vapor deposition of an inexpensive solution of DEZn in n-hexane (ca. 17 wt.%). The GZO films exhibited low resistivity (3.61  10–4 Ω cm) and high transmittance (85%) in the visible range. Interestingly, post-annealing treatment of the GZO films under N2 at 525 °C for just 10 min increased the number of carbon-interstitial oxygen defects (CZn+2Oi)〃, which played the role of acceptors and enhanced the film properties significantly. This approach potentially allows the fabrication of inexpensive transparent conducting oxides for use in solar cells.
    Moreover, we also explored the methodology to increase the light diffuse transmittance through controlling the preferred orientation of polycrystalline GZO films grown by the low-pressure chemical vapor deposition (LPCVD) technique. X-ray diffraction measurement indicated that major growth direction was (002) plane and secondary electron microscopy showed that column-like granule structure with planar surface was formed. By depositing a low temperature ZnO layer to serve as a template for high temperature GZO film growth, the main preferred orientation of the GZO films was manipulated to (110) plane and the film surface to the pyramid-like structure. Through this two-step growth, the light diffuse transmittance of the film with a GZO (800 nm)/ZnO (766 nm) combination exhibited 13% increase at 420 nm wavelength due to the preservation of the pyramidal surface morphology.

    Acknowledgments i Abstract ii Table of contents iv List of tables vii List of figures viii List of abbreviations xii Chapter 1 Introduction 1 1.1 Overview about Transparent Conducting Oxide (TCO) 1 1.2 The properties of TCO 2 1.2.1 Electrical properties 2 1.2.2 Optical properties 4 1.3 The major based-TCO materials 4 1.3.1 Indium-based TCO materials (ITO) 4 1.3.2 Tin Oxide (SnO2)-based TCO materials 6 1.3.3 Zinc Oxide-Based TCO materials 7 1.4 Fundamental and properties of ZnO 8 1.4.1 Introduction 8 1.4.2 Crystal structure 10 1.4.3 Lattice parameter 11 1.4.4 Electronic and band structure 12 1.4.5 Electrical properties 13 1.4.6 Doping in ZnO 13 1.4.7 Optical properties of ZnO 15 1.5 Thin Films Growth techniques 16 1.5.1 Chemical Vapor Deposition (CVD) Technique 16 1.5.2 Physical Vapor Deposition (PVD) Technique 17 1.5.3 Spin-coating film deposition process 18 1.6 The motivations and the aim of the present research 20 Chapter 2 Materials, Equipment and Characterization Techniques 24 2.1 Materials 24 2.1.1 Zinc precursors 24 2.1.2 Gallium precursor 24 2.1.3 Water (H2O) 25 2.1.4 Nitrogen (N2) 25 2.1.5 Substrate 25 2.1.6 Acetone 25 2.1.7 Ethanol 25 2.2 Metalorganic chemical vapor (MOCVD) deposition system 26 2.2.1 Pumping system 27 2.2.2 Heating system 27 2.2.3 Mass flow controller 27 2.2.4 Substrate preparation 27 2.3 Experimental procedures 27 2.3.1 Synthesis of GZO films using various Zn precursors 27 2.3.2 Experimental procedure for fabrication of GZO pyramidal texture surface 28 2.4 Thin Films Characterization Techniques 28 2.4.1 X-ray Diffraction (XRD) 28 2.4.2 Surface morphology and thickness of the films 29 2.4.3 Electron Spectroscopy for Chemical Analysis (ESCA)/ X-ray Photoelectron Spectroscopy (XPS) 30 2.4.4 Electrical Characterization of Films 31 2.4.4.1 Hall Measurement of thin films 31 2.4.4.2 Four-point probe measurement of thin films 34 2.4.5 UV-Visible Absorption Spectroscopy (UV-Vis) measurement 36 Chapter 3 Effects of zinc precursor on the properties of ZnO:Ga films prepared through metalorganic chemical vapor deposition 37 3.1 Back ground and motivation 37 3.2 Results and discussion 37 3.2.1 Effect of deposition temperature on the electrical properties of GZO film 37 3.2.2 Morphology and structure of synthesized GZO thin films prepared using the solution-based Zn precursor 38 3.2.3 Electrical and optical properties of synthesized GZO thin films prepared using the solution-based Zn precursor 41 3.2.4 Effect of annealing on properties of GZO thin films prepared using the solution-based Zn precursor 43 3.2.5 Effect of annealing on properties of GZO thin films prepared using the pure Zn precursor. 48 3.3 Conclusions 51 Chapter 4 Preferred orientation control of Ga doped ZnO films prepared through MOCVD for light scattering enhancement 52 4.1 Back ground and motivation 52 4.2 Results and discussion 53 4.2.1 Effect of growth temperature on the orientation of GZO films. 53 4.2.2 Effect of ZnO buffer layer thicknesses on the orientation of GZO films 54 4.3 Conclusions 61 Chapter 5 Conclusions 62 Supporting Information 64 References 66 List of publications 74 List of conference/seminar 75

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