The Electrical Characteristics of Aluminum-Doped Zinc Oxide Nanorods and p-Type Silicon Heterojunctions
莊家彰、李世鴻
E-mail: [email protected]
ABSTRACT
In this study, aluminum-doped zinc oxide (Al-doped ZnO) nanorods which were prepared with doping aluminum nitrate (Al(NO3)3 9H2O) by solution growth method on p-type silicon substrate were fully characterized. First, ethyl alcohol (C2H5OH) was added to zinc acetate (Zn(CH3COO)2 2H2O) to form a 0.0075M mixed solution. This mixed solution was then used to form a seeding layer on silicon substrate by spin coating. Subsequently, mixed solutions using 0.02M hexamethylenetetramine (C6H12N4), 0.02M zinc nitrate hexahydrate (Zn(NO3)2 6H2O), and aluminum nitrate (Al(NO3)3 9H2O) of various concentrations were prepared.
And the growth was carried out in the mixed solution at 90?C for two hours. As observed from field-emission scanning electron microscope (FE-SEM), the synthesized ZnO are hexagonal nanorods indeed. The chemical components of Al-doped ZnO nanorods were determined from energy diffraction spectroscopy (EDS) and are zinc, oxygen, and aluminum. The conductivity type for Al-doped ZnO nanorods is n-type indeed as was determined from Hall effect measurement, and the conductivity has been increased substantially by aluminum nitrate concentration; while mobility for majority carrier decreases with aluminum nitrate. As expected, the Al-doped ZnO nanorods prepared by aluminum nitrate of different concentrations also exhibit different I-V characteristics. In addition, the photoluminescence (PL) characteristic peak is in the range between 376.1nm and 379.4nm for Al-doped ZnO nanorods. Lastly, Al-doped ZnOnanorods were fabricated on a p-type silicon substrate to form a n-ZnO/p-Si heterojunction. This n-ZnO/p-Si heterojunction exhibits rectifying characteristics and its parameters such as reverse saturation current and ideality factor have been successfully determined.
Keywords : aluminum-doped zinc oxide (Al-doped ZnO)、Hall effect measurement、photoluminescence (PL)、n-ZnO/p-Si heterojunction
Table of Contents
封面內頁 簽名頁 中文摘要．．．．．．．．．．．．．．．．．．．．．．．．iii ABSTRACT．．．．．．．．．．．
．．．．．．．．．．．．v 誌謝．．．．．．．．．．．．．．．．．．．．．．．．．．vi 目錄．．．．．．．．．
．．．．．．．．．．．．．．．．．vii 圖目錄．．．．．．．．．．．．．．．．．．．．．．．．．x 表目錄．．．
．．．．．．．．．．．．．．．．．．．．．．xiv 第一章 緒論．．．．．．．．．．．．．．．．．．．．．1 1.1 氧 化鋅的歷史與簡介．．．．．．．．．．．．．1 1.2氧化鋅的特性．．．．．．．．．．．．．．．．3 1.3氧化鋅的摻雜
．．．．．．．．．．．．．．．．4 1.4氧化鋅的應用．．．．．．．．．．．．．．．6 1.5 研究動機．．．．．．．．
．．．．．．．．．8 第二章 氧化鋅奈米結構相關文獻回顧．．．．．．．．10 2.1以摻雜鋁製備氧化鋅奈米柱相關文獻
．．．．．．．．10 2.2以氧化鋅製作異質接面相關文獻．．．．．．．．．19 2.3以摻雜鋁製備氧化鋅之光學特性相關文 獻．．．．22 第三章 理論與研究方法．．．．．．．．．．．．．．25 3.1氧化鋅奈米柱的成長機制．．．．．．．．．
．．25 3.2氧化鋅摻雜．．．．．．．．．．．．．．．．．27 3.3 氧化鋅製備方法．．．．．．．．．．．．．．．27 3.3.1 水熱法．．．．．．．．．．．．．．．．．．28 3.3.2化學氣相沉積法(CVD)．．．．．．．．．．．29 3.3.3鋅蒸 氣氧化法．．．．．．．．．．．．．．．29 3.3.5 模板法．．．．．．．．．．．．．．．．．．30 3.4.實驗流程與步驟
．．．．．．．．．．．．．．．31 3.4.1 實驗流程．．．．．．．．．．．．．．．．．31 3.4.2 實驗基材與化學試劑．
．．．．．．．．．．．32 3.4.3 基板清洗．．．．．．．．．．．．．．．．．33 3.4.4 成長氧化鋅奈米柱．．．．．．
．．．．．．．33 3.4.5 高溫爐管退火．．．．．．．．．．．．．．．35 3.4.6 氧化鋅奈米柱電性量測．．．．．．．．
．．．35 3.5.實驗儀器與原理．．．．．．．．．．．．．．．36 3.5.1 場發射掃描式電子顯微鏡．．．．．．．．．．36 3.5.2 能量散佈分析儀．．．．．．．．．．．．．．36 3.5.3 霍爾效應量測．．．．．．．．．．．．．．．37 3.5.4 光激 發螢光校應量測．．．．．．．．．．．．45 3.5.5 pn接面特性．．．．．．．．．．．．．．．48 第四章 實驗結果與討 論．．．．．．．．．．．．．．．56 4.1 不同硝酸鋁濃度對氧化鋅奈米柱的研究與討論．．．56 4.1.1 氧化鋅奈米柱的表 面形貌(FE-SEM)之分析．．56 4.1.2 氧化鋅奈米柱的元素成份(EDS)之分析．．．．66 4.1.3 氧化鋅奈米柱的霍爾效應量測 之分析．．．．68 4.1.4 氧化鋅奈米柱的光激發螢光效應之分析．．．72 4.1.5 氧化鋅奈米柱的異質接面整流特性之分析．
．74 第五章結論．．．．．．．．．．．．．．．．．．．．．77 參考文獻．．．．．．．．．．．．．．．．．．．
．．．．79 圖目錄 圖1-1 (a) 氧化鋅纖鋅礦結構；(b)不同極性表面的氧化鋅結構模型．．．．．．．．．．．．．．．．．
．．．．．．2 圖2-1(a) 倍率30K奈米螺絲狀之氧化鋅結構；(b) 倍率55K奈米螺絲狀之氧化鋅結構；(c) 倍率15K奈米螺絲狀 之氧化鋅截面圖．．．．．．．．．．．．．．．．．．．．．12 圖2-2 (a) 奈米螺絲末端平面之HRTEM影像與EDS元素 分析，小圖為SAD選區電子繞射圖．．．．．．．．．．．．13 圖2-3 (a) 樣品一(無摻雜)；(b) 樣品二(摻雜1%)；(c) 樣品三(
摻雜3%)；(d) 樣品四(摻雜4%)之SEM圖，小圖為剖面圖。樣品一、二、三與四摻雜鋁所成長氧化鋅奈米柱高度分別 為120nm、110nm、90nm、及70nm，；另外隨著濃度不同其高度為0.70μm、1.20μm、1.45μm及1.75μm．．．．．
．15 圖2-4 (a) 樣品一、二、三及四之電阻率曲線圖；(b) 樣品一、二、三及四之載子濃度曲線圖．．．．．．．．．．．．
．17 圖2-5 樣品一、二、三及四在11K下所量測之PL光譜，在紫外區有微弱的激發現象能隙約3.32eV~3.34eV，另外 在1.96eV左右也有微弱的黃光．．．．．．．．．．．．．．．．18 圖2-6 n型氧化鋅與p型矽所結合成之異質接面之I-V特 性曲線及此元件結構示意圖．．．．．．．．．．．．．．．．20 圖2-7 (a)室溫下量測ZnO之PL譜；(b)室溫下量測ZnO 之EL譜．．．．．．．．．．．．．．．．．．．．．．21 圖2-8 (a) 以穿透式電子顯微鏡電子能量損失光譜
技(TEM-EELS)鋁元素於摻雜鋁氧化鋅奈米線的分佈；(b) 奈米線所對應的電子繞射圖；(c) 三種不同摻雜鋁元素的氧化鋅奈 米線於常溫下所得之陰極發光光譜．．．．．．．．．．．．．22 圖2-9 (a)~(c) 由濺鍍機成長的氧化鋅薄膜之 SEM 圖
；(d)~(f) 以合金氣相蒸鍍法將不同外觀的氧化鋅薄膜置於相同的成長位置所成長的摻雜鋁的氧化鋅奈米線之 SEM 圖．．．
．．．．．．．．．．．．．．．．．．．．24 圖3-1 圖3-1理想化的氧化鋅晶體在[0001]的界面結構圖像．．．．．．．
．．．．．．．．．．．．．．25 圖3-2 圖3-2理想氧化鋅柱狀成長．．．．．．．．．28 圖3-3 模板法．．．．．．．．
．．．．．．．．．．．．30 圖3-4 實驗流程圖．．．．．．．．．．．．．．．．．．31 圖3-5 場發射掃瞄式電子顯微 鏡(附EDS)．．．．．．．．39 圖3-6 白金蒸鍍機．．．．．．．．．．．．．．．．．．39 圖3-7 移動載子為電子之霍爾 效應．．．．．．．．．．．41 圖3-8移動載子為電洞之霍爾效應．．．．．．．．．．．．．41 圖3-9 霍爾效應量測儀 器．．．．．．．．．．．．．．．44 圖3-10 樣品放置載台．．．．．．．．．．．．．．．．．44 圖3-11 電子躍遷圖 示．．．．．．．．．．．．．．．．45 圖3-12 光激發螢光效應儀器示意圖．．．．．．．．．．．46 圖3-13 光激發螢 光效應儀器．．．．．．．．．．．．．．47 圖3-14 樣片激發之載台．．．．．．．．．．．．．．．．47 圖3-15 (a)簡 化的pn接面結構；(b)理想均勻摻雜的pn接面雜質濃度分佈．．．．．．．．．．．．．．．．．．．48 圖3-16 空間電荷 區、電場及電荷載子所受的作用力．．．．49 圖3-17 pn接面施加順向偏壓下之穩態少數載子濃度．．．．50 圖3-18 pn接 面空間電荷區中的電子電流密度及電洞電流密度．．．．．．．．．．．．．．．．．．．．．50 圖3-19 pn接面二極體 理想電流─電壓特性．．．．．．．．53 圖3-20 電流在對數座標下的理想pn接面二極體之I-V特性．．．．．．．．．．
．．．．．．．．．．．53 圖3-21 Keithley 237量測儀．．．．．．．．．．．．．．．54 圖3-22 製作完成之量測樣品．
．．．．．．．．．．．．．54 圖4-1 不同濃度硝酸鋁之摻雜鋁氧化鋅奈米柱之3K倍率FE-SEM上視圖，其中硝酸鋁濃度 分別為：(a) 0.00002M、(b) 0.00004M、(c) 0.00008M、(d) 0.00016M、(e) 0.0002M、(f) 0.0004M、(g) 0.0008M．．．．．．．
．．．．．．．59 圖4-2 不同濃度硝酸鋁之摻雜鋁氧化鋅奈米柱之30K倍率FE-SEM上視圖，其中硝酸鋁濃度分別為：(a) 0.00002M、(b) 0.00004M、(c) 0.00008M、(d) 0.00016M、(e) 0.0002M、(f) 0.0004M、(g) 0.0008M．．．．．．．．．．．．
．60 圖4-3 不同濃度硝酸鋁之摻雜鋁氧化鋅奈米柱之100K倍率FE-SEM上視圖，其中硝酸鋁濃度分別為：(a) 0.00002M、(b) 0.00004M、(c) 0.00008M、(d) 0.00016M、(e) 0.0002M、(f) 0.0004M、(g) 0.0008M．．．．．．．．．．．．．61 圖4-4 不同 濃度硝酸鋁之摻雜鋁氧化鋅奈米柱之7K倍率FE-SEM剖面圖，其中硝酸鋁濃度分別為：(a) 0.00002M、(b) 0.00004M、(c) 0.00008M、(d) 0.00016M、(e) 0.0002M、(f) 0.0004M、(g) 0.0008M．．．．．．．．．．．．．．62 圖4-5 不同濃度硝酸鋁 之摻雜鋁氧化鋅奈米柱之20K倍率FE-SEM剖面圖，其中硝酸鋁濃度分別為：(a) 0.00002M、(b) 0.00004M、(c) 0.00008M
、(d) 0.00016M、(e) 0.0002M、(f) 0.0004M、(g) 0.0008M．．．．．．．．．．．．．63 圖4-6 不同濃度硝酸鋁所成長之摻 雜鋁氧化鋅奈米柱之直徑關係圖．．．．．．．．．．．．．．．．．．．．．．64 圖4-7 不同濃度硝酸鋁所成長之摻雜 鋁氧化鋅奈米柱之高度關係圖．．．．．．．．．．．．．．．．．．．．．64 圖4-8 不同濃度硝酸鋁所成長之摻雜鋁之 元素百分比分佈圖．．．．．．．．．．．．．．．．．．．．．．．67 圖4-9 不同濃度硝酸鋁所成長之摻雜鋁氧化鋅奈 米柱之導電率關係圖．．．．．．．．．．．．．．．．．．．．．70 圖4-10 不同濃度硝酸鋁所成長之摻雜鋁氧化鋅奈 米柱之載子遷移率關係圖．．．．．．．．．．．．．．．．．．．．70 圖4-11 不同濃度硝酸鋁所成長之摻雜鋁氧化鋅 奈米柱之載子濃度關係圖．．．．．．．．．．．．．．．．．．．．71 圖4-12 不同濃度硝酸鋁所成長之摻雜鋁氧化鋅 奈米柱之PL關係圖．．．．．．．．．．．．．．．．．．．．．．72 圖4-13 不同濃度硝酸鋁所成長之摻雜鋁氧化鋅奈 米柱之介面電流關係圖．．．．．．．．．．．．．．．．．．．．74 圖4-14 不同濃度硝酸鋁所成長之摻雜鋁氧化鋅奈 米柱對數電流─電壓關係圖．．．．．．．．．．．．．．．．．．76 表目錄 表1-1 氧化鋅的基本性質．．．．．．．．
．．．．．．．．．2 表3-1 本實驗製備之基板．．．．．．．．．．．．．．．32 表3-2 本實驗製備之藥品．．．．．．
．．．．．．．．．32 表4-1 不同濃度硝酸鋁所成長之摻雜鋁氧化鋅奈米柱之直徑、高度與高寬比關係表．．．．．．．
．．．．．．．．．．65 表4-2 不同濃度硝酸鋁所成長之摻雜鋁氧化鋅奈米柱之元素百分比分佈圖．．．．．．．．．．
．．．．．．．．．66 表4-3 不同濃度硝酸鋁所成長之摻雜鋁氧化鋅奈米柱之霍爾效應量測關係圖．．．．．．．．．．
．．．．．．．．．69 表4-4 不同濃度硝酸鋁所成長之摻雜鋁氧化鋅奈米柱之多數載子(電子)濃度關係圖．．．．．．．
．．．．．．．．．71 表4-5 不同濃度硝酸鋁所成長之摻雜鋁氧化鋅奈米柱之PL波長關係圖．．．．．．．．．．．．．
．．．．．．．．．73 表4-6 不同濃度硝酸鋁所成長之摻雜鋁氧化鋅奈米柱之逆向飽和電流及理想因子．．．．．．．．
．．．．．．．．76
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