本研究發展出簡單且高再現性的製程提升鑽石的場發射特性及穩定性，我們發展出三種方式來達成：第一，利用矽基板當基底，製作矽尖端結構並沉積複合式鑽石薄膜(奈米微晶鑽石薄膜/超奈米微晶鑽石薄膜)。第二，結合奈米碳管和鑽石薄膜，不僅降低起始電場且提升場發射的電流密度，穩定性測試也提升此碳材料的使用壽命。第三，利用高導電率之鑽石薄膜，進一步修飾超奈米微晶鑽石薄膜於奈米碳管之微結構，使之形成高導電率的針狀結構薄膜，且增進場發射特性。其相關的可能機制也將被探討。
本研究一主題旨在探討提升場發射特性之發射源之製程。為了製備場發射源，我們藉由兩段式微波電漿輔助化學氣相法沉積複合式鑽石薄膜於矽金字塔模版。從穿透式電子顯微鏡影像圖顯示此複合式鑽石薄膜之組成為存在大量的石墨相於大顆鑽石晶粒周圍且小顆的鑽石晶粒圍繞於晶界附近。因此說明此複合式鑽石薄膜擁有良好的場發射特性，其主要由獨特的薄膜微結構所貢獻。
本研究另一主題為結合奈米碳管與鑽石薄膜用以增進場發射穩定性探討其微結構和表面形貌。利用複合式鑽石薄膜沉積於預鍍奈米鑽石顆粒之奈米碳管-矽基底，不僅延長奈米碳管為基底的使用壽命且提升了場發射性質。其奈米碳管扮演的角色為抑制了鑽石薄膜與矽基底之界面的非晶碳形成，且有效的使矽基底之電子穿越過界面到鑽石薄膜；複合式鑽石薄膜富含小鑽石晶粒和石墨相。綜合這兩項因素，此複合式鑽石薄膜/奈米碳管之發射源有助於增強場發射特性。
本研究最後發展出高導電奈米微晶鑽石薄膜與奈米碳管結合之“奈米複合碳材”場發射材料，方法之一是奈米碳管之改質，以便在其上以甲烷/氮氣電漿成長具有針狀結構之高導電奈米微晶鑽石薄膜；方法之二是利用低溫偏壓輔助法在甲烷/氮氣電漿後處理製程將超奈米微晶鑽石薄膜/奈米碳管之鑽石晶粒改為針狀奈米晶，大幅提升發射體之導電性及場發射特性。藉由穿透式電子顯微鏡詳細探討其微結構之變化，並利用此材料製作三極式場發射電晶體。

Growth, microstructure and electron field emission (EFE) characteristics of diamond films were investigated in this research work. A facile and reproducible way was developed to enhance the stability of EFE properties of diamond films. Firstly, hybrid granular structured diamond (HiD) films, which were nanocrystalline diamond/ultrananocrystalline diamond (UNCD) films, were coated on Si tips by a two-step microwave plasma enhanced chemical vapor deposition (MPE-CVD) process to synthesize the high performance EFE emitters. Secondly, the integration of the diamond films with high robustness and the carbon nanotubes (CNTs) with marvelous EFE properties that yielded highly stable electron sources was demonstrated. Lastly, high conductivity diamond-graphite nano-carbon composite (DGC) films were utilized to modify the granular structure of UNCD/CNTs films to form needle-like diamond grains encased in nano-graphitic layers, which possess high conductivity and improve EFE properties. The feasible mechanisms will be discussed.
In the development of the nano-EFE emitters via the preparation of HiD on Si tip templates using a two-step MPE-CVD process, the mechanism which improved EFE properties were investigated. The superior EFE properties of the HiD films can be attributed to the formation of unique granular structure of the films. The transmission electron microscopic investigations revealed that the HiD films consisted of abundant graphitic phases, which were located at the periphery of large diamond aggregates and at the boundaries between the ultra-small diamond grains.
The development of the CNTs-based EFE emitters, the enhanced lifetime stability for the CNTs by coating HiD films on nanodiamond particulates decorated CNTs/Si-based emitters using a two-step MPE-CVD process was reported, overcoming the drawback of short lifetime of the CNTs-based EFE-emitters. The use of CNTs effectively suppresses the presence of amorphous carbon in the diamond-to-Si interface that enhances the transport of electrons from Si, across the interface, to diamond. The two-step MPE-CVD process results in the coalescence of the small grains in UNCD films and the formation of abundant graphitic phases in these films. All these factors contribute toward the enhancement on the EFE process for the HiD/CNTs/Si-based emitters.
Finally, we integrated high conductivity DGC films and CNTs and demonstrated the potential applications for EFE emitters as well as triode vacuum field emission transistor. The growth of high conductivity DGC films on CNTs were achieved by (i) strengthening the CNTs for directly growth of DGC films on CNTs in CH4/N2 plasma and (ii) lower growth temperature for DGC films by bias-enhanced plasma post-treatment process.

中文摘要………………………………………………………………………………I
Abstract……………………………………………………………………………..III
Acknowledgement…………………………………………………………………V
Outline………………………………………………………………………............VI
Table List…………………………………….……………………………...……….X
Figure List…………………………………………………………………..............XI
Acronyms and abbreviations………………………………………...…………..XXI
Chapter 1 Overview
1.1 Background………………………………………………………………………1
1.2 Motivation………………………………………………………………………..2
1.3 Organization of the thesis…………………………………………………...…..3
Chapter 2 Literature review
2.1 Introduction to diamond films…………………….…..………………….......4
2.1.1 Diamond synthesis…………………………………………………...…..…..7
2.1.2 Diamond nucleation…………………………..………………………...…..10
2.1.3 Growth of UNCD films…...……………………………..…………………..11
2.1.4 Electron field emission theory……………………………..……………….....12
2.1.5 Electron field emission of diamond films……………………………...……..14
2.1.6 Fabrication of diamond field emitters………………....................................17
2.2 Introduction to CNTs……………………………………………….………...18
2.2.1 CNTs synthesis…………………………..…………………………………....19
2.2.2 Structure of CNTs……………………………………………………………..20
2.2.3 Electron field emission of CNTs……………………………………………...22
2.3 Field emission applications…………………………………………………24
2.4 Aim of this investigation…………………………………………………....25
Chapter 3 Experimental procedures and characterizations
3.1 Fabrication Si-tip structures……………………………...…………………27
3.2 Synthesis of CNTs……………………………………..………...………..27
3.2.1 Synthesis of conventional CNTs………………...……………..……...……….27
3.2.2 Synthesis of strengthen CNTs (s-CNTs)……………..….…………………......28
3.3 Synthesis of diamond films………...…………………………...……………..28
3.3.1 Synthesis of UNCD films……………………...……….………………...…...28
3.3.2 Synthesis of HiD films……………………………………………………..…29
3.3.3 Synthesis of DGC1 films (I): direct CH4/N2 plasma grow on s-CNTs or Si substrate……………………………………………………………...………..29
3.3.4 Synthesis of DGC2 films (II): plasma post-treatment (ppt) of UNCD film...29
3.4 Characterization of diamond films………...…………………........................30
3.4.1 Field emission scanning electron microscope (FESEM)……………………30
3.4.2 Raman spectroscopy…………………………………………………………..30
3.4.3 X-ray photoemission spectroscopy (XPS)……………………………………31
3.4.4 Near-edge X-ray absorption fine structure (NEXAFS) spectroscopy……...…31
3.4.5 Transmission electron microscope (TEM)……………………………………31
3.4.6 Electron field emission and microplasma measurement……………………33
Chapter 4 Enhancing the electron field emission and plasma illumination behavior using hybrid diamond emitters
4.1 Research background…………………………………….…………...……….35
4.2 Results and discussion………...………………….………….………………...37
4.2.1 The characteristics of UNCD films grown on Si-tip arrays…….…………......37
4.2.2 The characteristics of HiD films grown on Si-tip arrays…….........................48
4.2.3 TEM microstructure investigation……………………………………………..53
4.3 Summary………………………….……………………………………….…...57
Chapter 5 Role of carbon nanotube interlayer in enhancing the electron field emission behavior of ultrananocrystalline diamond films
5.1 Research background…….…………………………………………...……….58
5.2 Results and discussion (I)---Diamond coated CNTs…….…………...………60
5.2.1 Materials characterization……………………………………..…..……….....60
5.2.2 TEM microstructure investigation………………..……………………...…...65
5.2.3 Electron field emission and plasma illumination studies……………………..69
5.2.4 Summary………………….……………..………………………………..…..77
5.3 Results and discussion (II)---Diamond coated CNTs/Si-tip arrays…….…78
5.3.1 Materials characterization…………………………..…………..………...…78
5.3.2 Electron field emission and plasma illumination studies..….……...…………81
5.3.3 TEM microstructure investigation………………………………...……..….88
5.3.4 Summary…………………….………………………………………...……...95
Chapter 6 High stability electron field emitters synthesized via the combination of carbon nanotubes and diamond-graphite nano-carbon composite films
6.1 Research background…………..…………………..…………………….…....97
6.2 Results and discussion (I)---Strengthening the CNTs for growing DGC1 on CNTs……………………………………….………………………………….100
6.2.1 Characterizations of s-CNTs nanostructures……………………………...…100
6.2.2 Characterizations of Diamond Films Grown on s-CNTs…………………....106
6.2.3 TEM microstructure investigation……………………….…………….…....110
6.2.4 Electron field emission and plasma illumination studies…............................118
6.2.5 Summary……………………….…………………………………...…….....128
6.3 Results and discussion (II)---Plasma post-treatment of UNCD films for growing DGC2 on CNTs………………………...…………………………...128
6.3.1 Materials characterizations………..…………………………………………128
6.3.2 TEM microstructure investigation…….……………………………….……132
6.3.3 Electron field emission study………………….………….…………………136
6.3.4 Summary…………………………………………………………….………137
Chapter 7 The applications of high conductivity and superior electron field emission materials for flexible EFE emitters and triode vacuum field emission transistor
7.1 Research background………………………….……………………………..139
7.2 Results and discussion…………………..………………………………..…142
7.2.1 Characterization and analysis of the DGC2 films for flexible EFE emitters...142
7.2.2 Characterization and analysis of the diamond/CNTs-based triode VFE transistor………..…………………………………………………………147
7.3 Summary……………………………...………………..……..………………151
Chapter 8 Conclusions and perspective
8.1 Conclusions………………………………………………………………….153
8.2 Perspective……………………………………………………………….154
References………………………………………………………………………….156
Publications………………………………………………………………………..178

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