本研究在三種氣體條件下，以負偏壓成長(Bias Enhanced Growth, BEG)製程，在施加偏壓成核與成長過程中，會利用光放射光譜(Optic Emission Spectroscopy, OES)與偏壓電流(Bias Current)監測製程，並利用拉曼(Raman)光譜、SEM 分析表面形貌、本研究有三種不同實驗條件，(1)甲烷/氫氣電漿：固定成長時間30分鐘、微波功率、甲烷/氫氣比例，改變偏壓值，腔室壓力，希望可以在氫氣電漿下控制其鑽石晶粒尺寸大小，使其擁有UNCD的鑽石晶粒大小，以期改善其場發射特性。(2)甲烷/氫氣/氬氣電漿：我們在第一部分的實驗中，找一組有較佳的場發射特性的條件，在甲烷/氫氣電漿中加入不同比例氬氣，觀察其結果變化。(3)甲烷/氬氣電漿：第三部份我們嘗試在一般成長UNCD的條件下，用偏壓輔助成長鑽石膜，觀察場發射特性變化。由穿透式電子顯微鏡(Transmission Electron Microscopy，TEM)的觀察發現電子場發射特性變佳的主要因素是在 U-BEG過程中成長鑽石薄膜會沿著晶界處產生石墨相。

In this thesis, we used U-BEG(ultrasonication-bias enhanced growth) in three different Experimental conditions. In applying a bias nucleation and growth process will profit OES (optic Emission Spectroscopy)  and bias current monitoring process and utilize Raman spectroscopy, SEM(scanning electron microscope) analysis of surface morphology, electronic EFE (field emission) measurements feature diamond films. Investigate how changes in field emission property.

目錄
致謝…………………………………………………………………I
中文摘要…………………………………………………………II
英文摘要…………………………………………………………III
目錄………………………………………………………………IV
圖目錄………………………………………………………………V
表目錄……………………………………………………………VI
第一章序論	..............................1
1.1 研究動機	..............................1
1.2 鑽石的基本特性	......................1
1.2.1 硬度(Hardness)：	......................1
1.2.2 熱傳導係數(Thermal conductivity)：......2
1.2.3 化學反應性(Chemical reactivity)：	......2
1.2.4 密度(Density)：	......................2
1.2.5 光學性質(Optical properties)﹕	......2
1.2.6 電子特性﹕	......................2
1.2.7 鑽石的負電子親和力特性:	..............2
1.3 微米及超奈米晶鑽石薄膜之合成方法與理論....2
1.3.1 合成鑽石薄膜之方法	..............2
1.3.2 鑽石薄膜成核相關理論	..............3
1.4 鑽石薄膜在場發射特性上之應用	......8
1.5 微米及超奈米晶鑽石薄膜之應用	......9
第二章 實驗方法	.............................25
2.1 薄膜製備	.............................25
2.1.1 實驗設備與方法	.....................25
2.1.1.1實驗設備	.............................25
2.2 薄膜物性量測	.....................28
2.2.1 拉曼光譜	.............................29
2.2.2 掃描式電子顯微鏡(圖 2.5)	.............30
2.2.3 電子場發射	.....................31
2.2.4 穿透式電子顯微鏡(圖 2.8)	.............35
第三章 結果與討論	.....................48
3.1甲烷/氫氣電漿成長鑽石膜	.............48
3.1.1掃描式電子顯微結構分析	.............49
3.1.2 沉積速率分析	.....................49
3.1.3 拉曼光譜分析	.....................49
3.1.4 電子場發射分析	.....................49
3.1.5 偏壓電流分析	.....................50
3.1.6 小結	.............................50
3.2在氫氣電漿中加入氬氣取代部分氫氣成長鑽石膜	...50
3.2.1掃描式電子顯微結構分析	.............51
3.2.2 沉積速率分析	.....................51
3.2.3 拉曼光譜分析	.....................51
3.2.4 電子場發射分析	.....................51
3.2.5 偏壓電流分析	.....................51
3.2.6 小結	.............................51
3.3 甲烷/氬氣電漿中加偏壓輔助成長鑽石膜	.....52
3.3.1掃描式電子顯微結構分析	.............52
3.3.2 沉積速率分析	.....................52
3.3.3 拉曼光譜分析	.....................52
3.3.4 電子場發射分析	.....................53
3.3.5 偏壓電流分析	.....................53
3.3.6小結	.............................53
3.4實驗結果比較	.............................53
3.4.1掃描式電子顯微結構分析	.............54
3.4.2沉積速率	.............................54
3.4.3 拉曼光譜分析	.....................54
3.4.4 電子場發射分析	.....................54
3.4.5 TEM 穿透式電子顯微鏡分析	.............54
第四章 結論與未來展望	.....................98
參考文獻	............................100
圖目錄
圖  1-1鑽石的結構[15]	.....................14
圖  1-2石墨的結構[16]	.....................14
圖  1-3微米晶至超奈米晶鑽石薄膜表面型態......15
圖  1-4 HRTEM 分析超奈米晶鑽石晶粒及晶界[15].16
圖  1-5超奈米晶鑽石晶粒間距及繞射圖[16]	.....16
圖  1-6同波長的超奈米晶鑽石膜拉圖曼光譜[19]..17
圖  1-7微波電漿 CVD 示意圖[21]	.............17
圖  1-8 HRTEM 分析超奈米晶鑽石晶粒及晶界[15].18
圖  1-9微波電漿放電系統示意圖[23]	.....18
圖  1-10射頻電漿放電系統示意圖[24]	.....19
圖  1-11電子迴旋共振微波放電示意圖[25]	.....19
圖  1-12鑽石之椅狀堆積構造[26]	.............20
圖  1-13石墨及鑽石的活化能相對圖[27]	.....20
圖  1-14薄膜與基材之早期成核方式	.....21
圖  1-15與基材不反應者之孕核、成長	.....21
圖  1-16偏壓輔助孕核法的反應機制[38]	.....22
圖  1-17偏壓輔助成核示意圖[41]	.............23
圖  1-18超音波振盪法及偏壓輔助孕核法成長鑽石薄膜之 SEM 圖[47]	.....................................23
圖  1-19分別運用奈米鑽石粉(ND)和奈米鑽石粉+鈦粉(ND + Ti)以超音波振盪法成長不同時間之 UNCD]	.............24
圖  2-1 IPLAS, CYRANNUS® I 微波電漿化學汽相沉積系統示意圖：	.....................................37
圖  2-2本研究所採用MPECVD：IPLAS, CYRANNUS® I	...38
圖  2-3偏壓系統示意圖	...........................38
圖  2-4 (a)拉曼光譜(Raman spectra：RENISHAW®, INVIA)系統，	...........................................39
圖  2-5(a) 掃描式電子顯微結構系統(Scanning Electron	..41
圖  2-6電子場發射(EFE)特性量測系統	..................42
圖  2-7金屬-真空能帶示意圖(a)未加電場，(b)外加高電場[51]	...........................................43
圖  2-8碳原子 sp3 結構圖(a)cubic Diamond(c-D)，(b)new	.45
圖  2-9穿透式電子顯微鏡(TEM：JEOL, JEM-2100F)	.........46
圖  2-10穿透式電子顯微鏡(TEM：JEOL, JEM-2100F)的基本構造示意圖 [57]	............................................47
圖  3-1 1400 W 35 torr 甲烷9%之光放射光譜	....56
圖  3-2 1400 W 40 torr 甲烷9%之光放射光譜	....57
圖  3-3 1400 W 45 torr 甲烷9%之光放射光譜	....57
圖  3-4 1400 W 50 torr 甲烷9%之光放射光譜	....58
圖  3-5 1400W  35torr 甲烷 9%之偏壓電流	............58
圖  3-6 1400W  40torr 甲烷 9%之偏壓電流	............59
圖  3-7 1400W  45torr 甲烷 9%之偏壓電流	............59
圖  3-8 1400W  50torr 甲烷 9%之偏壓電流	............60
圖  3-9 1400W 35torr CH4 9% 之SEM圖	............60
圖  3-10 1400W 40torr CH4 9% 之SEM圖	............61
圖  3-11 1400W 45torr CH4 9% 之SEM圖	............61
圖  3-12 1400W 50torr CH4 9% 之SEM圖	............62
圖  3-13 1400W CH4 9% 偏壓-沉積速率圖	............64
圖  3-14 1400W 35torr CH4 9% 鑽石膜沉積厚度之SEM圖	.64
圖  3-15 1400W 40torr CH4 9% 鑽石膜沉積厚度之SEM圖	.65
圖  3-16 1400W 45torr CH4 9% 鑽石膜沉積厚度之SEM圖	.65
圖  3-17 1400W 50torr CH4 9% 鑽石膜沉積厚度之SEM圖	.66
圖  3-18 1400 W 35torr 甲烷9%之拉曼光譜圖	.........66
圖  3-19 1400 W 40torr 甲烷9%之拉曼光譜圖	.........67
圖  3-20 1400 W 45torr 甲烷9%之拉曼光譜圖	.........67
圖  3-21 1400 W 50torr 甲烷9%之拉曼光譜圖	.........68
圖  3-22 1400W CH4 9% 負偏壓-場發射值圖	.................70
圖  3-23 1400W 35torr 之電子場發射J-E 曲線	.........70
圖  3-24  1400W 40torr 之電子場發射J-E 曲線	.........71
圖  3-25 1400W 45torr 之電子場發射J-E 曲線	.........71
圖  3-26 1400W 50torr 之電子場發射J-E 曲線	.........72
圖  3-27 不同氫氣/氬氣量之光放射光譜	.................73
圖  3-28 1400W 40torr不同氫氣/氬氣量之偏壓電流	.........74
圖  3-29 1400W 40torr 不同氫氣/氬氣量之SEM圖	.........74
圖  3-30 不同氫氣/氬氣比例之負偏壓-沉積速率	.........75
圖  3-31 不同氬氣量成長鑽石膜沉積厚度之SEM圖	.........76
圖  3-32 1400 W 40torr  Ar 15%之拉曼光譜圖	.........76
圖  3-33 1400 W 40torr Ar 30%之拉曼光譜	.................77
圖  3-34 1400 W 40torr Ar 45%之拉曼光譜	.................77
圖  3-35 1400W 4torr Ar 15% 之電子場發射J-E 曲線	.78
圖  3-36 1400W 4torr Ar 30% 之電子場發射J-E 曲線	.79
圖  3-37 1400W 4torr Ar 45% 之電子場發射J-E 曲線	.79
圖  3-38 1000W 150 torr 2% CH4之光放射光譜	.........80
圖  3-39 1000W 150 torr 3% CH4之光放射光譜	.........81
圖  3-40 1000W 150 torr 4% CH4之光放射光譜	.........81
圖  3-41 1000W 1500torr CH4 2% 之偏壓電流	.........82
圖  3-42 1000W 1500torr CH4 3% 之偏壓電流	.........82
圖  3-43 1000W 1500torr CH4 4% 之偏壓電流	.........83
圖  3-44 1000W 150torr CH4 2% 之SEM圖	.................83
圖  3-45 1000W 150torr CH4 3% 之SEM圖	.................84
圖  3-46 1000W 150torr CH4 4% 之SEM圖	.................84
圖  3-47 1000 W 150torr CH4 2%之拉曼光譜	.........85
圖  3-48 1000 W 150torr CH4 3%之拉曼光譜	.........85
圖  3-49 1000 W 150torr CH4 4%之拉曼光譜	.........86
圖  3-50 甲烷濃度-負偏壓之沉積速率圖	.................87
圖  3-51 不同甲烷濃度-偏壓成長鑽石膜沉積厚度之SEM圖	.88
圖  3-52 甲烷濃度-起始電場之場發射值圖	.................89
圖  3-53 1000W 150torr CH4 2% 之電子場發射J-E 曲線	.90
圖  3-54 1000W 150torr CH4 3% 之電子場發射J-E 曲線	.90
圖  3-55 1000W 150torr CH4 4% 之電子場發射J-E 曲線	.91
圖  3-56偏壓 -200V不同實驗條件之SEM圖	.................92
圖  3-57偏壓 -200V不同實驗條件之Raman圖	.................92
圖  3-58偏壓-200V 不同氣體條件成長鑽石膜之TEM與HR明場像	.93
圖  3-59偏壓-200V 甲烷/氫氣成長鑽石膜之TEM HR	.........93
圖  3-60偏壓-200V 甲烷/氫氣成長鑽石膜之TEM HR	.........94
圖  3-61偏壓-200V 甲烷/氫氣成長鑽石膜之TEM HR	.........94
圖  3-62偏壓-200V 甲烷/氫氣/氬氣成長鑽石膜之TEM HR	.95
圖  3-63偏壓-200V 甲烷/氫氣/氬氣成長鑽石膜之TEM HR	.95
圖  3-64偏壓-200V 甲烷/氫氣/氬氣成長鑽石膜之TEM HR	.96
圖  3-65偏壓-200V 甲烷/氬氣成長鑽石膜之TEM HR	.........96
圖  3-66偏壓-200V 甲烷/氬氣成長鑽石膜之TEM HR	.........97 
表目錄
表 1-1鑽石的基本特性………………………………………………12
表 1-2微米晶鑽石與超奈米晶鑽石的特性比較[14] ………………13
表 1-3超音波振盪法以及偏壓輔助孕核法其孕核特性之比較[47]
       …………………………………………………………………13
表 2-1碳結構的各種拉曼峰值…………………………………40
表 2-2碳原子 sp3 結構 1/d 值與其出現之晶相對照表[58]…………44
表 3-1 1400W CH4 9%改變偏壓、氣壓之實驗參數…………………56
表 3-2 1400W CH4 9% 之實驗參數與鑽石膜沉積速率…………63
表 3-3 1400W CH4 9% 之實驗參數與電子場發射起始電場.........69
表 3-4 改變氬氣比例之實驗參數…………………………………73
表 3-5 改變氬氣比例之實驗參數與沉積速率……………………75
表 3-6 1400W 40torr改變氬氣量之實驗參數與電子場發射起始電場
   ………………………………………………………………………78
表 3-7 1000W 150torr 之實驗參數…………………………………80
表 3-8 1000W 150torr改變氣體比之實驗參數與沉積速率…………87
表 3-9 1000W 150torr改變氣體比之實驗參數與電子場發射起始電場
       ………………………………………………………………89

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