由於奈米碳管具備異向性質，為整合運用於各類元件並正確利用其異向性，必須於適當圖案位置上控制其方向，以獲得預期功能與效率。本論文研究電漿化學氣相沉積奈米碳管成長、方向性控制及組裝，其目的為開發成長過程中與成長後之碳管方向性及圖案組裝技術。除於成長過程中提供含鈦物種，定性探討低溫成長機制外，並以電漿中電場特性搭配觸媒奈米點製造技術，控制奈米碳管成長方向及位置，探討影響方向性成長及有序陣列成長的原因；此外，並分別以磁場及水分子毛細力組裝碳管排列方向與薄膜圖案型態，瞭解相關組裝機制與特性，以符合奈米碳管應用需求。
本研究所獲結論概述如下：在TiCl4/CH4/H2/N2電漿氣氛下，無觸媒之空白基板上可沉積TiCN鍍層，但於含鎳觸媒之基板上，僅藉觸媒輔助成長奈米碳管，表面則有含鈦非晶質層沉積。此同軸結構及觸媒電子繞射分析顯示鈦原子無法溶入觸媒並擴散析出。鈦與碳原子於鎳觸媒顆粒中之選擇性溶解與擴散差異，可證實本研究於580℃成長碳管時，觸媒顆粒仍維持固態。
可藉簡易之鞘層電場控制技術，操控單支離散奈米碳管(或纖維)的順向成長方向。鞘層中固定方向的電場可使碳管(或纖維)沿其方向順向排列成長，因此，於鞘層範圍內調整試片傾斜角度，碳管可組裝形成不同預定的排列方向。但成長高密度束狀碳管時則無法改變排列方向，傾斜基板上之束狀碳管仍垂直基板表面成長，其順向機制由高密度碳管間的凡得瓦力主導，而非電場控制。
在中空陰極電漿下，可獲得特殊且呈對稱方向成長的碳纖維型態，其原因為中空陰極電漿於基材表面施予特殊電場分佈所致。由於電場反轉特性，兩種順向成長趨勢共存，沿中空陰極橫軸方向之碳纖維為收斂方向成長，縱軸方向則呈現發散型態。
利用外加磁場組裝已成長之順向奈米碳管，並探討其組裝機制，其中碳管一端含殘留觸媒顆粒。由碳管薄膜之磁滯曲線鑑定，搭配觸媒顆粒的晶體方向分析，可確認碳管平行磁場方向排列的原因為頂端鐵磁顆粒之形狀磁異向性，而非由觸媒本質之晶體磁異向性產生。
結合奈米壓印技術製備週期性鎳奈米點，可成長有序碳管陣列。由於TiN中介層具低表面能，成長時圖案奈米點傾向分裂為更小顆粒，造成小直徑碳管團簇成長而降低有序程度。然而，可藉改變成長氣氛以調整觸媒的表面張力而避免分裂，達成有序成長。
最後提出以浸潤自組裝方式改善碳管薄膜之場發射性質。起始電場由組裝前5.75 V/μm降低至組裝後2.5 V/μm，其原因為潤濕後之碳管薄膜組裝為尖錐圖案型態，降低屏蔽效應。

To properly utilize the anisotropic properties of carbon nanotubes (CNTs) in device applications, the control of the CNT orientations on patterned positions is a necessity since this would largely determine the device funtionality and performance. The growth, orientation control, and related assembly of CNTs are explored in this study. The main purposes are to develop the direct-growth and post-growth assembly techniques to achieve orientation control and patterning. The growth mechanism of CNTs is qualitatively examined by simultaneously supplying Ti species for CNT growth. By employing the physical characteristics of electric fields in plasma and the fabrication of catalyst dots, the directional and patterned growth of CNTs are investigated. In addition, the self-assemblies of the CNT orientations and arrangemnts by external magnetic fields and capillary forces respectively are also described.
Under a TiCl4/CH4/H2/N2 plasma ambient, a continuous TiCN film is formed in the absence of catalysts; however, only CNTs are grown through the catalytic vapor growth, with the amorphous Ti-containing layers coated on their surfaces. The obtained coaxial structure and the electron diffraction analysis of catalysts support that Ti atoms hardly dissolve into the catalyst and pass through it. Selective dissolution and diffusion between the Ti and C atoms in Ni nanoparticles suggest that catalysts during the growth of CNTs at 580oC are in solid state.
The aligned growth of isolated CNTs and carbon nanofibers (CNFs) via a simple sheath-dependent technique for orientation control is demonstrated. The electric field within the plasma sheath contributes to the aligned growth with an absolute orientation, and can be used to direct the assembly of CNTs/ CNFs in a predetermined manner relative to the substrate by tilting the sample in a sheath region. However, the alignment of high-density CNT bundles grown on inclined substrates is always perpendicular to the surfaces. The alignment mechanism of CNT bundles is dominated by the van der Waals forces even under the electric fields.
CNFs with specific and symmetrically aligned configurations are grown on a flat surface during hollow cathode discharge (HCD). The alignment results from a unique electric field distribution imposed on the substrate surface in the HCD environment. Due to the field reversal characteristic, two alignment trends simultaneously occur. For the transverse direction of the channel, the grown CNFs on the substrate appear in a convergent manner, while those along the longitudinal direction exhibit a radiative arrangement.
Magnetic post-assembly of aligned CNTs only having catalyst nanoparticles capped at one end and the related assembly mechanisms are described. The reason why the CNT orientation aligns parallel to the field direction is mainly attributed to the magnetic shape anisotropy rather than the crystalline anisotropy, of the encapsulated ferromagnetic nanoparticle, based on the identification of the hysteresis loops for the as-grown CNT films as well as the analysis of the relative crystal orientations of catalysts with respect to the alignment axis.
Ordered arrays of aligned CNTs are grown from periodic arrays of Ni dots defined by nanoimprint lithography. Due to the low surface energy of the TiN interlayers employed, the patterned Ni dots tend to break into smaller nanoparticles during growth, thus resulting in the growth of smaller diameter nanotubes and the decrease in ordering. However, by adjusting the growth conditions with consequent modification of the surface tension of catalysts, isolated ordered CNT arrays can be prepared without the occurrence of catalyst breaking.
Finally, a wetting-induced self-assembly strategy is proposed to enhance the field emission properties of CNT films.�n The turn-on field reduces from 5.75 V/μm (for the as-grown CNT films) to 2.5 V/μm (for the re-arranged CNTs), where the improvement arises from the reduction of screening effect since the CNT films are assembled into patterned tower-like structures.

中文摘要 Ⅰ
英文摘要 Ⅲ
誌謝 Ⅴ
總目錄 Ⅵ
表目錄 Ⅸ
圖目錄 Ⅹ
中英名詞與符號對照表 ⅩⅦ
第一章 緒論 1
第二章 理論基礎與文獻回顧 5
2-1 電漿原理 5
2-1-1 電漿化學與特性 5
2-1-2 電漿輔助化學氣相沉積 6
2-1-3 中空陰極電漿 7
2-2 奈米碳管結構與電性關係 8
2-2-1 單壁奈米碳管 8
2-2-2 多壁奈米碳管 10
2-3 奈米碳管氣相成長機制 10
2-3-1 頂部與底部成長模式 11
2-3-2 碳原子擴散路徑 12
2-3-3 擴散驅動力 12
2-4 電場輔助奈米碳管順向成長 13
2-5 奈米壓印技術 16
2-6 電子場發射特性 17
第三章 實驗方法與步驟 20
3-1 實驗流程 20
3-2 電漿化學氣相沉積系統設備 21
3-3 材料的選用 23
3-3-1 反應氣體 23
3-3-2 基板材料 23
3-3-3 製備觸媒之材料 23
3-3-4 壓印用材料 24
3-4 實驗參數與步驟 24
3-4-1 觸媒製備 24
3-4-2 電漿化學氣相沉積法成長奈米碳管 24
3-4-1 3-4-3 奈米碳管低溫成長機制研究 26
3-4-4 以外加磁場組裝奈米碳管 26
3-5 奈米碳管的分析與鑑定 27
第四章 奈米碳管低溫成長機構 30
4-1 前言 30
4-2 成長氣氛中TiCl4添加的效應 31
4-3 觸媒物理狀態的推測 37
第五章 直接成長組裝 40
--- 控制奈米碳管成長方向與位置
5-1 前言 40
5-2 以鞘層電場控制奈米碳管成長方向 42
5-2-1 鞘層中成長行為及方向性控制 42
5-2-2 改變碳管成長方向 49
5-2-3 束狀碳管於電漿環境中順向成長機制 51
5-2-4 方向性碳管偏極化拉曼分析 57
5-2-5 碳管排列方向對場發射性質之影響 57
5-3 中空陰極電漿方向性成長奈米碳纖維 61
5-4 結合奈米壓印技術成長有序碳管陣列 75
5-4-1 點狀圖案觸媒與碳管陣列製備 76
5-4-2 氣氛與基材表面能對成長碳管陣列的影響 81
5-4-3 高度/間距比值對場發射性質的影響 84
第六章 成長後組裝 88
--- 奈米碳管的方向性排列與薄膜型態組裝
6-1 前言 88
6-2 以外加磁場組裝含觸媒顆粒之奈米碳管 88
6-2-1 磁場與觸媒顆粒存在與否對組裝的影響 90
6-2-2 觸媒顆粒易磁化方向及方向性排列機制 95
6-2-3 磁組裝碳管之電性 103
6-3 奈米碳管浸潤自組裝 110
6-3-1 碳管薄膜潤濕特性 110
6-2-1 浸潤自組裝圖案對場發射性質之影響 114
第七章 總結論 119
參考文獻 121
自述 131
著作 131

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