臺灣博碩士論文加值系統

本實驗使用P-Si(100)基板，以射頻磁控濺鍍法將三氧化二鋁（Al2O3）薄膜以及氧化鋅種子層(ZnO seed)沉積在基板上，接下來再以低溫水溶液合成法成長一維氧化鋅奈米柱，探討不同水溶液濃度以及不同成長時間下，利用掃描式電子顯微鏡、X-ray繞射分析儀、光激發螢光光譜、CIE色座標、I-V曲線等，分析不同尺寸大小的奈米柱結構變化對光學特性的影響。
本實驗所製作之電激發光元件架構為ITO/ZnO nanorods/ZnO seed/
Al2O3/P+-Si/Al，低溫水溶液合成法所使用材料分別為為六甲基四胺(C6H12N4)與二水合醋酸鋅(Zn(CH3COO)2)，將其粉末與水溶液混和後，在90℃的環境氛圍下，以不同濃度以及不同成長時間合成一維氧化鋅奈米柱，用以探討一維氧化鋅奈米柱對於氧化鋅薄膜之電激發光元件之光學影響。
本實驗分別以0.01M、0.02M、0.03M三種水溶液濃度，各別沉積30、60、90以及120分鐘來去探討不同尺寸大小的奈米柱對光學的影響以及找出最佳化的參數，從實驗各項數據來看0.03M 水溶液中成長60分鐘之元件，有最佳的發光強度，伴隨著沉積時間越久，鋅間隙和氧空位比例大幅提升，可見光波長強度越來越強，主波長會逐漸漂移至可見光波長。

In this experiment, P-Si(100) is used mainly as substrate, after deposit Al2O3 thin film and ZnO seed layer on the substrate by RF magnetron sputtering method. Then, grow one dimensional ZnO nanorods by used low temperature aqueous solution meth, by exploring vary with concentration and grown time of aqueous solution, and take advantage of methods such as scanning electron microscope, X-ray diffractometer, photoluminescence spectrum, CIE chromaticity coordinate, I-V curve, etc., the influence of the variety of the structure of ZnO nanorods on the optical property then different size analysis.
The architecture of electroluminescence device prepared by this experiment is ITO/ZnO nanorods/ZnO seed/ Al2O3/P+-Si/Al, C6H12N4 and Zn(CH3COO)2 are used material in low temperature aqueous solution meth respectively, after mixed the two powders and aqueous solution, under the environment atmosphere of 90℃, synthesis one dimensional ZnO nanorods by different concentration and different grown time, in order to investigate the optical property influences of ZnO thin film electroluminescence device of one dimensional ZnO nanorods.
In this experiment, three different concentration of aqueous solution be used by 0.01M 0.02M and 0.03M, Individual growth time is 30min 60min 90min and 120min to investigate the effect of sizes of nanorods optical property influences and find out optimization parameters,
from the experiment data, the device of 0.03M aqueous solution with growth time is 60min have better luminescence intensity. With the growth time is longer, interstitial Zn and oxygen vacancies ratio will be increase substantially and visible wavelength intensity will more and more, main-wavelength will shift gradually towards visible wavelength.

目錄
摘要 I
Abstract II
目次 Ⅲ
表目次 Ⅵ
圖目次 VII
Chapter 1 緒論 1
1-1 發光二極體種類 2
1-2 直、交流薄膜電激發光元件特點 3
1-2.1直、交流薄膜電激發光元件的優缺點 3
1-2.2氧化鋅薄膜電激發光元件製程展望 3
1-3 研究動機與目的 4
1-4 論文架構 4
Chapter 2 理論分析與文獻回顧 5
2-1 奈米材料發展與簡介 5
2-1.1尺寸效應 6
2-1.2表面效應 6
2-1.3庫倫堵塞效應 7
2-1.4量子穿隧效應 7
2-1.5量子限域效應 7
2-2 電激發光元件結構與發光原理 8
2-3 電激發光元件各層材料的擇優選擇 9
2-3.1基板 9
2-3.2絕緣層 9
2-3.3螢光層 10
2-3.4透明導電薄膜 11
2-3.5金屬電極 12
2-4 電激發光機制 12
2-4.1直接撞擊激發 12
2-4.2能量轉移原理 12
2-5 發光層薄膜 13
2-5.1 發光材料介紹 13
2-5.2 氧化鋅薄膜結構 13
2-5.3 氧化鋅薄膜發光機制 14
2-5.3.1 紫外光(Ultraviolet, UV) 14
2-5.3.2 綠光(Green) 14
2-5.3.3 黃橙光(Yellow-orange) 15
2-6 各類氧化鋅奈米結構合成方法介紹 15
2-7 低溫水溶液合成法成長一維氧化鋅奈米柱 16
2-8 磁控濺鍍與電漿原理 17
2-9 微影製程介紹 17
2-10薄膜成型機制 18
Chapter 3 實驗方法與步驟 19
3-1 矽基板清洗 19
3-2 高溫硼擴散 19
3-3 氧化鋅奈米柱電激發光元件製備 20
3-3.1 濺鍍步驟及參數 20
3-3.2 低溫水溶液合成法成長氧化鋅奈米柱 20
3-3.3 熱退火處理 21
3-3.4 光罩之設計 21
3-3.5 黃光微影製程 21
3-3.6 背電極沉積 21
3-4 特性量測 22
3-4.1 掃描式電子顯微鏡(Hitachi S4800) 22
3-4.2 X-ray繞射分析儀(BRUKER, D2 PHASER) 22
3-4.3 原子力顯微鏡((NTMDT P47H)表面分析 23
3-4.4 光激發光(He-Cd Laser 325nm)特性分析 23
3-4.5 電激發光(Spectrometer BRC111A)特性分析 24
3-4.6 電壓電流曲線(凱思隆-電壓電流量測追蹤曲線儀)特性分析 24
Chapter 4 實驗結果與分析 25
4-1 掃描式電子顯微鏡表面型態分析(SEM) 25
4-2 X-ray繞射分析儀(XRD) 26
4-3原子力顯微鏡表面型態分析(AFM) 26
4-4光激發螢光光譜(PL) 27
4-5電激發光光譜(EL) 28
4-6 CIE色坐標 28
4-7 I-V特性曲線 29
4-8電激發光元件施加偏壓後實際點亮之照片 29
Chapter 5 結論 31
Reference 32

表目錄
Table 2-1 二氧化矽與三氧化二鋁介電係數與介電崩潰電場 41
Table 2-2 氧化鋅基本特性簡介 42
Table 3-1 不同材料濺鍍參數 55
Table 3-2 各種顯微鏡比較 55
 
圖目錄
Fig. 1-1不同驅動電壓電激發光元件種類圖 41
Fig. 2-1不同尺寸氧化鋅奈米柱光激發光光譜，a、b、c 直徑分別為 100nm、50nm、25nm之奈米柱 43
Fig. 2-2 (a)金屬與半導體能量-能階密度關係圖(b)不同維度之能階密度-能量函數關係圖 43
Fig. 2-3 單絕緣層直流電激發光元件架構圖(A)基板(B)絕緣層(C)發光層(D)上電極(E)背電極 44
Fig. 2-4 雙絕緣層交流電激發光元件架構圖 44
Fig. 2-5單絕緣層電激發光元件元件內部等效電路 45
Fig. 2-6光波長與光子關係圖 45
Fig. 2-7 雙絕緣薄膜電激發光元件能帶圖 46
Fig. 2-8 氧化鋅六方纖鋅礦結構 46
Fig. 2-9 E. G. Bylander 等人所提出氧化鋅缺陷能階圖 47
Fig. 2-10 B. Lin 等人所提出氧化鋅缺陷能階圖 47
Fig. 2-11 Zheng-Wu Jin 等人文獻中氧化鋅摻銅的陰極發光光譜圖 48
Fig. 2-12異質成核示意圖 48
Fig. 2-13氧化鋅結晶成長結構 49
Fig. 2-14一維氧化鋅奈米柱成長過程示意圖 49
Fig. 2-15不同 PH 濃度成長氧化鋅奈米尺寸示意圖 50
Fig. 2-16濺鍍原理示意圖 50
Fig. 2-17薄膜成長過程(a)粒子成核(b)晶粒成長(c)晶粒聚結(d)縫隙填補(e)薄膜成長 51
Fig. 2-18濺鍍法沉積薄膜其不同結構區域俯視圖 51
Fig. 2-19濺鍍法沉積薄膜其不同結構區域橫截面圖 52
Fig. 3-1 氧化鋅奈米柱電激發光元件製備流程圖 53
Fig. 3-2 10mm*10mm 電極光罩設計圖 54
Fig. 3-3 布拉格晶格原理 55
Fig. 3-4 電子傳輸轉移圖 55
Fig. 3-5 光激發光量測系統架構 56
Fig. 3-6 電激發光量測系統架構 56
Fig. 4-1 濃度0.01M成長30分鐘(a)倍率30K(b)倍率80K 57
Fig. 4-2 濃度0.01M成長60分鐘(a)倍率30K(b)倍率80K 58
Fig. 4-3 濃度0.01M成長90分鐘(a)倍率30K(b)倍率80K 58
Fig. 4-4 濃度0.01M成長120分鐘(a)倍率30K(b)倍率80K 59
Fig. 4-5 濃度0.02M成長30分鐘(a)倍率30K(b)倍率80K 60
Fig. 4-6 濃度0.02M成長60分鐘(a)倍率30K(b)倍率80K 60
Fig. 4-7 濃度0.02M成長90分鐘(a)倍率30K(b)倍率80K 61
Fig. 4-8 濃度0.02M成長120分鐘(a)倍率30K(b)倍率80K 62
Fig. 4-9 濃度0.03M成長30分鐘(a)倍率30K(b)倍率80K 62
Fig. 4-10濃度0.03M成長60分鐘(a)倍率30K(b)倍率80K 63
Fig. 4-11濃度0.03M成長90分鐘(a)倍率30K(b)倍率80K 64
Fig. 4-12濃度0.03M成長120分鐘(a)倍率30K(b)倍率80K 64
Fig. 4-13 Al2O3薄膜XRD分析圖 65
Fig. 4-14 低溫水溶液濃度0.01M成長(a)30分鐘(b)60分鐘(c)90分鐘(d)120分鐘 XRD分析以及(e)各繞射峰值強度比較 66
Fig. 4-15 低溫水溶液濃度0.02M成長(a)30分鐘(b)60分鐘(c)90分鐘(d)120分鐘 XRD分析以及(e)各繞射峰值強度比較 68
Fig. 4-16 低溫水溶液濃度0.03M成長(a)30分鐘(b)60分鐘(c)90分鐘(d)120 分鐘 XRD分析以及(e)各繞射峰值強度比較 70
Fig. 4-17 低溫水溶液濃度為0.01M成長30分鐘之AFM表面粗糙度分析 71
Fig. 4-18 低溫水溶液濃度為0.01M成長60分鐘之AFM表面粗糙度分析 72
Fig. 4-19 低溫水溶液濃度為0.01M成長90分鐘之AFM表面粗糙度分析 73
Fig. 4-20 低溫水溶液濃度為0.01M成長120分鐘之AFM表面粗糙度分析 74
Fig. 4-21 低溫水溶液濃度為0.02M成長30分鐘之AFM表面粗糙度分析 75
Fig. 4-22 低溫水溶液濃度為0.02M成長60分鐘之AFM表面粗糙度分析 76
Fig. 4-23 低溫水溶液濃度為0.02M成長90分鐘之AFM表面粗糙度分析 77
Fig. 4-24 低溫水溶液濃度為0.02M成長120分鐘之AFM表面粗糙度分析 78
Fig. 4-25 低溫水溶液濃度為0.03M成長30分鐘之AFM表面粗糙度分析 79
Fig. 4-26 低溫水溶液濃度為0.03M成長60分鐘之AFM表面粗糙度分析 80
Fig. 4-27 低溫水溶液濃度為0.03M成長90分鐘之AFM表面粗糙度分析 81
Fig. 4-28 低溫水溶液濃度為0.03M成長120分鐘之AFM表面粗糙度分析 82
Fig. 4-29 低溫水溶液濃度為0.01M、0.02M及0.03M成長30 ~ 120分鐘之 AFM Rrms趨勢圖 82
Fig. 4-30 低溫水溶液濃度為0.01M成長(a)30分鐘(b)60分鐘(c)90分鐘(d)120分鐘(e)30~120分鐘全部之PL分析 84
Fig. 4-31 低溫水溶液濃度為0.02M成長(a)30分鐘(b)60分鐘(c)90分鐘(d)120分鐘(e)30~120分鐘全部之PL分析 86
Fig. 4-32 低溫水溶液濃度為0.03M成長(a)30分鐘(b)60分鐘(c)90分鐘(d)120分鐘(e)30~120分鐘全部之PL分析 87
Fig. 4-33 低溫水溶液濃度為0.01M成長(a)30分鐘(b)60分鐘(c)90分鐘(d)120分鐘(e)30~120分鐘全部之EL量測 89
Fig. 4-34 低溫水溶液濃度為0.02M成長(a)30分鐘(b)60分鐘(c)90分鐘(d)120分鐘(e)30~120分鐘全部之EL量測 91
Fig. 4-35 低溫水溶液濃度為0.03M成長(a)30分鐘(b)60分鐘(c)90分鐘(d)120分鐘(e)30~120分鐘全部之EL量測 92
Fig. 4-36 低溫水溶液濃度為0.01M成長(a)30分鐘(b)60分鐘(c)90分鐘(d)120分鐘CIE色座標 94
Fig. 4-37 低溫水溶液濃度為0.02M成長(a)30分鐘(b)60分鐘(c)90分鐘(d)120分鐘CIE色座標 95
Fig. 4-38 低溫水溶液濃度為0.03M成長(a)30分鐘(b)60分鐘(c)90分鐘(d)120分鐘CIE色座標 97
Fig. 4-39 低溫水溶液濃度為0.03M成長30~120分鐘之氧化鋅奈米柱電激發光元件電壓-電流特性曲線 97
Fig. 4-40 低溫水溶液濃度為0.01M成長30分鐘之電激發光元件施加15V電壓實際點亮照片 98
Fig. 4-41 低溫水溶液濃度為0.01M成長60分鐘之電激發光元件施加15V電壓實際點亮照片 98
Fig. 4-42 低溫水溶液濃度為0.01M成長90分鐘之電激發光元件施加15V電壓實際點亮照片 99
Fig. 4-43 低溫水溶液濃度為0.01M成長120分鐘之電激發光元件施加15V電壓實際點亮照片 99
Fig. 4-44 低溫水溶液濃度為0.02M成長30分鐘之電激發光元件施加15V電壓實際點亮照片 100
Fig. 4-45 低溫水溶液濃度為0.02M成長60分鐘之電激發光元件施加15V電壓實際點亮照片 100
Fig. 4-46低溫水溶液濃度為0.02M成長90分鐘之電激發光元件施加15V電壓實際點亮照片 101
Fig. 4-47 低溫水溶液濃度為0.02M成長120分鐘之電激發光元件施加15V電壓實際點亮照片 101
Fig. 4-48低溫水溶液濃度為0.03M成長30分鐘之電激發光元件施加15V電壓實際點亮照片 102
Fig. 4-49低溫水溶液濃度為0.03M成長60分鐘之電激發光元件施加15V電壓實際點亮照片 102
Fig. 4-50低溫水溶液濃度為0.03M成長90分鐘之電激發光元件施加15V電壓實際點亮照片 103
Fig. 4-51低溫水溶液濃度為0.03M成長120分鐘之電激發光元件施加15V電壓實際點亮照片 103

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