臺灣博碩士論文加值系統

奈米碳管為新興之半導體材料，頗具研究價值，本論文研究內容涵蓋三個大方向，包含: (1) 多壁奈米碳管氣體感測器之研製，(2) 多壁奈米碳管場發射之研製，(3) 選擇性提取半導體性單壁奈米碳管與場效電晶體之研製。其個別之研究結果如下所述:
在本文的開頭，我們首先研究成長高密度的多壁奈米碳管，經由電子顯微鏡觀察到平均長度和平均直徑分別為：4.52 um 與 45 nm。第一部分，藉由金屬奈米粒子吸附於奈米碳管表面作為氣體感測之研究。根據氣體感測量測結果發現奈米銀粒子吸附明顯增加感測器的靈敏度。在室溫下通入800 ppm 異丙醇氣體量測，結果發現靈敏度提高至5.31％，並且具有高度穩定性以及快速的反應。此外，本研究提出新方法，將高密度奈米碳管從矽基板轉移至可撓基板上，製作可撓性奈米碳管感測器。利用此轉移方法能夠增加碳管與可撓基板附著力，即使在極端的曲率半徑 933 um 下仍然保持高度的延展性。根據氣體感測量測結果，在奈米碳管表面吸附奈米金粒子，感測器表現出高的靈敏度、穩定性、重現性以及快速的響應，由此結果表明出可撓式奈米碳管氣體感測器的可行性，這將成為更具商業化的潛力。
第二部分，藉由金屬奈米粒子吸附於奈米碳管表面作為場發射之研究。由於奈米碳管具有極小的尖端曲率與高縱橫比，加上藉由金屬觸媒粒子吸附於奈米碳管表面，將可有效的降低材料功函數增進場發射最佳起始電場與臨界電場 J-E 與 I-V 特性。根據場發射量測結果，當發射電流密度達到 10 μA/cm2 下，啟始電場由純碳管的 5.33 V下降到金摻雜碳管的 4.84 V直到銀摻雜碳管的 3.94 V。金屬吸附奈米碳管增強的場發射性能的主要原因是較低的有效功函數。此外，本研究提出新方法，將高密度奈米碳管由矽基板轉移至可撓基板上，製作可撓性奈米碳管場發射元件。根據場發射量測結果，將可撓基板重覆彎曲至曲率半徑5 mm 下經過100次後，啟始電場分別為：3.60 V/μm 與 3.72 V/μm。由此結果表明出奈米碳管具有良好的機械穩定性。
第三部分，使用高品質的單壁奈米碳管，藉由分離的方式將半導體性奈米碳管從中提取，主要利用聚合物poly(3-dodecylthiophene) (rr-P3DDT)對半導體性的奈米碳管會產生包覆的特性並且排斥金屬性的奈米碳管，因此將其離心後可提取半導體性的奈米碳管。根據拉曼光譜分析結果，顯示出成功的分離出半導體性奈米碳管。我們使用分離過後的純半導體性奈米碳管做為場效電晶體主動層，該元件表現出高的開關比為107，次臨界擺幅為154 mV/dec。本研究所提出的方法能夠有效分離出半導體性奈米碳管，對於未來商業化有相當大的潛力，並且適合大面積電子設備使用。

In this study, the growth of high-density multi-wall nanotubes (MWNTs) on oxidized Si substrate was investigated. The obtained average length and diameter of the CNTs were approximately 4.52 and 45 nm, respectively. The adsorption of metal nanoparticle on nanotube surfaces and the fabrication of MWNT-based gas sensors were also examined. Ag adsorption to the MWNTs significantly increased device sensitivity and provided a 5.31% increase in RT sensitivity over that of MWNTs for an ambient isopropyl alcohol gas concentration of 800 ppm. The response speed and stability of the fabricated sensor were favorable. Moreover, the direct transfer of high-density MWNTs from a SiO2/Si substrate to a flexible substrate was demonstrated. The strong adhesion of the MWNTs with the flexible substrate was maintained although the substrate was bent into an extreme state with a radius of curvature of 993 μm. The surface modification of the MWNT-networked films with size-controlled Au nanoclusters enhanced gas sensitivity. The flexible MWNT sensor exhibited reproducibility, fast response, high stability, and high sensitivity. Results demonstrate the feasibility of manufacturing flexible MWNT gas sensors using the transfer process. This finding represents a major step toward low-cost and large-scale production of this class of device.
The measurements of MWNT-based field emission show that a low turn-on electric field with the emission current density of 10 μA/cm2 could be achieved because of metal adsorption. The measured values of Eto for Au- and Ag-coated MWNTs were 5.33, 4.84, and 3.94 V/μm. The comparative investigation indicates that Ag nanoparticle decoration on MWNT decreased work function from 5 eV to 3.94 eV. The enhanced field emission properties of metal-coated MWNTs were caused mainly by low effective work function. The flexible field emission with MWNT thin films was fabricated using a transfer method. In the turn-on electric field with emission current density of 10 μA/cm2, the measured values of Eto with and without bending test were 3.60 and 3.72 V/μm. The MWNT film showed good mechanical stability at a significantly small bending radius of 5 mm. The good mechanical bendability is due to the cracking-resistant nanotube morphology. A simple method for selectively separating semiconducting SWNTs (s-SWNTs) was developed. The samples were examined by Raman spectroscopy with an excitation laser of 633 and 785 nm wavelengths. The spectrum reveals that metallic SWNTs and regioregular poly(3-dodecylthiophene) were completely removed and s-SWNTs were remained. SWNT-based field-effect transistors (FETs) were fabricated by dip-coating method. The device with selective extraction had a high on/off ratio and low subthreshold swing. The transistor with selective extraction had an on/off ratio of 107 and a subthreshold swing of 154 mV/dec. The proposed convenient and effective s-SWNT sorting process can be used in the commercial manufacturing of SWNT-based FETs for low-cost and large-scale electronic devices.

Contents
摘要 I
Abstract IV
Acknowledgement VII
Contents VIII
Table Captions XI
Figure Captions XII

Chapter 1 Introduction
1-1 Background 1
1-2 Basic properties of CNT 2
1-3 Electronic Properties 3
1-4 Organization of this dissertation 3

Chapter 2 Methods for Synthesizing MWNTs
2-1 Growth Mechanism for MWNTs 12
2-2 Arc discharge 12
2-3 Laser ablation 13
2-4 CVD 13
2-5 Raman Spectroscopy of CNTs 13
2-6 Experimental details and analytic 14

Chapter 3 Application of CNTs in gas sensor
3-1 Introduction 22
3-2 Enhanced carbon nanotubes gas sensor with adsorbed metal nanoparticles 23
3-3 Flexible gas sensors with MWNTs thin films by using a simple transfer method 29
3-4 Summary 35
Chapter 4 Improved field emission properties of metal-decorated multi-walled carbon nanotubes
4-1 Introduction 66
4-2 Experiments 68
4-3 Results and discussion 69
4-4 Field emission based on MWNT thin films by a simple transfer method on flexible substrate 71
4-5 Summary 73

Chapter 5 Field-Effect Transistor Properties of Semiconducting Single Walled Carbon Nanotubes by Selective Extraction
5-1 Introduction 85
5-2 SWNTs Schottky contact 87
5-3 The fabrication of SWNTs FET 87
5-4 The Raman analysis of SWNTs 89
5-5 The field-effect transistor characteristics of SWNTs 91
5-6 Summary 93

Chapter 6 Conclusions and Future Work
6-1 Conclusions 103
6-2 Future work 105
Reference 106

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