一維鎵摻雜氧化鋅奈米塔: 晶體成長機制至性質與應用

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研究生：	邱顯明 Chiu, Hsien-Ming
論文名稱：	一維鎵摻雜氧化鋅奈米塔: 晶體成長機制至性質與應用 One-dimensional Gallium-doped Zinc Oxide Nanopagodas: From Growth Mechanism to Properties and Applications
指導教授：	吳振名 Wu, Jenn-Ming
口試委員:	吳振名裘性天吳文偉朱英豪李奕賢
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：	2014
畢業學年度：	102
語文別：	英文
論文頁數：	191
中文關鍵詞：	氧化鋅、金屬-有機化學氣相沉積法、奈米結構、p-n同質接面、光催化
外文關鍵詞：	ZnO, MOCVD, nanostructures, p-n homojunctions, photocatalysis
相關次數：	點閱：2 下載：0
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氧化鋅是II–VI族n型半導體，也是追求下一個世代電子和光子奈米元件用來取代矽的好候選材料之一。一維奈米結構，例如線、柱、管、環、帶、針，由於其獨特的性質，例如高寬高比與大表面積，在製造電子、光學、光電、電化學奈米元件上是相當好的材料。在本研究中，我們成功地利用金屬-有機化學氣相沉積法在鎵摻雜氧化鋅種子層/矽基板上製造出具有大面積、良好垂直性、單晶結構的鎵摻雜氧化鋅奈米塔陣列結構。
我們發現鎵原子在奈米柱側面晶面將{1-100}轉化成兩組({11-21}, {11-2-2})和({-2201}, {-110-1})，最後形成塔狀結構，扮演著一極重要的關鍵角色。經由理論模擬計算的結果得知，鎵原子可以降低({11-21}, {11-2-2})和({-2201}, {-110-1})的表面能；然而會增加{1-100}的表面能。此外，我們提出一個新的成長模型，藉由理論模擬計算在鎵摻雜後改變表面能的結果，來解釋如何從平滑的奈米柱{1-100}平面轉化成具皺褶狀的奈米塔({11-21}, {11-2-2})和({-2201}, {-110-1})平面。根據低溫陰極發光和光激發光光譜得知，鎵摻雜氧化鋅奈米塔擁有極好的晶體品質。
暴露晶面的種類強烈的影響其性質與表面活性。我們也研究了鎵摻雜氧化鋅奈米塔與氧化鋅奈米線其光電性質與其化學反應性。紫外光光偵測器的反應結果證明鎵摻雜氧化鋅奈米塔比氧化鋅奈米線不但具有更快速的電子-電洞產生與再結合速率，也同時具有更好的光催化活性。鎵摻雜氧化鋅奈米塔增進其效能是因為{11-21}, {11-22}, {-2201}, {-1101}平面相較於{10-10}和{11-20}平面更能增強氧氣和水的化學吸附活性。
為了追求高注入電流效率二極體奈米元件，全一維共軸氧化鋅p-n同質接面奈米結構是其中一種理想結構。我們將p型銀摻雜氧化鋅奈米結構殼包覆在n型鎵摻雜氧化鋅奈米塔核上，合成出全一維共軸氧化鋅p-n同質接面二極體。全一維的p-n銀-鎵摻雜氧化鋅和銀摻雜氧化鋅-氧化鋅共軸奈米結構相較於全二維或二維-一維p-n同質和/或異質接面二極體，具有更優秀的二極體特性表現，如更低開啟電場、更好的整流效率與理想因子。藉由低溫和變溫光激發光光譜技術分別可測得鎵和銀的束縛能。另比較銀-鎵摻雜氧化鋅又比銀摻雜氧化鋅-氧化鋅p-n同質接面奈米結構表現出更好的二極體特性。
最後，利用原子層沉積法沉積白金奈米粒子在一維鎵摻雜氧化鋅奈米塔上形成白金/鎵摻雜氧化鋅奈米複材。沉積上去的白金奈米粒子比傳統的濕化學法好，均勻且分散很好的分佈在鎵摻雜氧化鋅奈米塔表面上。白金/鎵摻雜氧化鋅奈米複材在30個原子層沉積循環時有顯著的改善光催化活性，在波長254奈米的紫外光照射下，其催化活性比純鎵摻雜氧化鋅奈米塔大約增加了2.7倍。我們從各種光催化機制去探討白金奈米粒子對光催化活性的影響。由於修飾的白金奈米粒子在光學吸收/穿透、電子-電動對分離/再結合、與區域表面電漿共振有競爭效應，因此，在白金奈米粒子含量上有一個最佳值，可以使一維白金/鎵摻雜氧化鋅奈米複材達到一個最大的光催化活性。
從基礎晶體成長機制研究到多方面的嶄新奈米元件應用，例如場發射子、單根奈米線場效電晶體、紫外光光偵測器、與光觸媒，鎵摻雜氧化鋅奈米塔比純氧化鋅奈米線具備更好的效果與性質。鎵摻雜氧化鋅奈米塔提供了一個追求下一個世代奈米元件應用上更好的另一種選擇平台。

Contents    I
Abstract    VI
摘要    IX

Chapter 1: Introduction I: Nanotechnology, Nanoscience, and Nanomaterials
1 Nanotechnology, nanoscience, and nanomaterials    1
2 Features of nanomaterials    3
2.1 Quantum tunnelling effect    3
2.2 Quantum confinement effect    3
2.3 Quantisation of energy    4
2.4 Surface effect    5
2.5 Coulomb blockade    6

Chapter 2: Introduction II: Zinc Oxide – Properties and Applications
1 Crystal structure, chemical bonding, and basic properties    15
1.1 Crystal structure    15
1.2 Chemical bonding    16
1.3 Basic properties    16
2 Synthesis of 1D ZnO nanostructures    16
2.1 Strategies for achieving 1D growth    17
2.2 Chemical vapor deposition (CVD)    17
2.3 Metal-organic chemical vapor deposition (MOCVD)    19
2.4 Molecular beam epitaxy (MBE)    19
2.5 Pulsed laser deposition (PLD)    20
2.6 Aqueous chemical growth (ACG) (or Hydrothermal)    20
2.7 Electrodeposition    21
3 N- and p-type doping of ZnO    22
3.1 N-type doping of ZnO    22
3.2 P-type doping of ZnO    23
4 Optical properties and defect chemistry of ZnO    24
4.1 Optical properties of ZnO    24
4.1.1 Free excitons and polaritons    25
4.1.2 Bound excitons    26
4.1.3 Two-electron satellites (TES)    27
4.1.4 Donor-acceptor-pair (DAP) and longitudinal optical (LO)-phonon replicas    27
4.2 Defect chemistry of ZnO    28
5 Applications of 1D ZnO nanostructures    29
5.1 Field emitter    29
5.2 Photo- and gas sensors    30
5.3 Diodes and light-emitting diodes (LED)    30
5.4 Laser    31
5.5 Solar cells    32

Chapter 3: Experimental Procedures
1 Deposition of GZO seed layer    53
2 Growth of GZO nanostructures    53
3 Characteristic measurements    54
3.1 Structure and morphology analysis    54
3.1.1 Scanning electron microscope (SEM)    54
3.1.2 (Scanning) transmission electron microscope (TEM/STEM)    55
3.1.3 X-ray diffraction (XRD)    56
3.2 Chemical composition and binding state analysis    56
3.2.1 Energy dispersive X-ray spectroscopy (EDS)    56
3.2.2 Auger electron spectroscopy (AES)    57
3.2.3 X-ray photoelectron spectroscopy (XPS)    57
3.3 Optical and electrical properties    58
3.3.1 Cathodoluminescence (CL) and photoluminescence (PL)    58
3.3.2 Electrical measurements    58

Chapter 4: Experimental and Computational Insights in the Growth of Gallium-Doped Zinc Oxide Nanostructures with Superior Field Emission Properties
1 Introduction    61
2 Experimental Procedures    63
2.1 Electrical measurements of GZO and ZnO nanostructures    63
2.2 Computational simulation    64
3 Results and Discussion    64
3.1 The effects of the growth temperature on GZO nanostructures    64
3.2 The effects of the Ga/Zn molar ratios on GZO nanostructures    66
3.3 The time evolution and spatial epitaxial orientation of the GZO nanostructures    68
3.4 Computational simulation of surface energies of GZO nanostructures    73
3.5 Optical and electrical properties of GZO nanostructures    74
4 Conclusions    78

Chapter 5: Opto-Electrical Properties and Chemisorption Reactivity of Ga-doped ZnO Nanopagodas
1 Introduction    94
2 Experimental Procedures    96
2.1 Electrical transport properties measured by three-terminal SWFET devices    96
2.2 Opto-electrical response of two-terminal UV PD devices    97
2.3 Photocatalytic activity of GZO and ZnO nanostructures array    97
3 Results and Discussion    97
3.1 Morphologies of ZnO NWs and GZO NPGs    98
3.2 Electrical transport properties of GZO NPGs    99
3.3 Opto-electrical properties of ZnO NWs and GZO NPGs    101
3.4 Photocatalytic activity of ZnO NWs and GZO NPGs    105
3.5 Chemisorption reactivity of ZnO NWs and GZO NPGs crystal planes    108
4 Conclusions    112

Chapter 6: Synthesis and Characterization of One-Dimensional Ag-doped ZnO/Ga-doped ZnO Coaxial Nanostructure Diodes
1 Introduction    125
2 Experimental Procedures    127
2.1 Growth and characterization of SZO-GZO coaxial core-shell nanostructures    127
2.2 Electrical properties of two-terminal SZO-GZO coaxial core-shell nanodevices    128
3 Results and Discussion    128
4 Conclusions    139

Chapter 7: Fabrication and Characterization of Well-dispersed Plasmonic Pt Nanoparticles on Ga-doped ZnO Nanopagodas Array with Enhanced Photocatalytic Activity
1 Introduction    148
2 Experimental Procedures    150
2.1 Decoration of Pt NPs    150
2.2 Photocatalytic activities of Pt/GZO hybrid nanocomposites    151
3 Results and Discussion    151
3.1 Characteristics of Pt/GZO hybrid nanocomposites    151
3.2 Photocatalytic activities of Pt/GZO hybrid nanocomposites    154
3.3 Photocatalytic mechanisms of Pt/GZO hybrid nanocomposites    157
4 Conclusions    163

Chapter 8: Conclusions    175

References:    178

                                

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