臺灣博碩士論文加值系統

　　在本論文中，藉由鎵參雜之氧化鋅薄膜作為緩衝層(buffer layer)，成功的藉由VLS (Vapor-Liquid-Solid)技術將單晶氧化鋅(Zinc Oxide)奈米線之(nanowires)奈米線垂直生成於玻璃基板上。我們在600°C的成長溫度中，成功的控制了奈米線的選區成長，並且所成長的奈米線，其直徑及長度都相當的均勻。經由(XRD)的檢驗，氧化鋅奈米線只有出現在(002)的面，以及極小的半高寬。為了尋求更精密的檢定，我們將試片送至高解析穿透式電子顯微鏡(HRTEM)和室溫及變溫的PL(photoluminescence spectroscopy)量測，證明其結晶性、垂直性都相當的優良。進行電子場發射(field electron emission)的實驗，在電場14V/μm開始，就有明顯的場發射電流存在，而在電流密度0.1 mA/cm2時，其電壓只需24 V/μm，故我們深信氧化鋅具有場發射應用的潛力。隨後我們在較低溫的成長溫度520°C下，於ZnO:Ga/glass基板上成長出一樣垂直單晶的氧化鋅奈米線，其長度約2.0μm，直徑約70-150nm，其結構一樣是單晶的wurtzite structure，經由UV光來照射，發現照射光的電流值約為暗室電流植的67.5倍。

　　高密度、垂直的氧化鋅奈米線選區成長於ZnO:Ga/Si3N4/SiO2/Si基板上，在採用兩階段的氧氣注入方式下，採用不同成長溫度來成長。可以很容易發現期間尖端為六角柱，當生成溫度越高時，其奈米線長度也跟著增加，但尖端的直徑卻隨之減少，故我們稱在500°C的奈米線形狀為管狀，而700°C所成長的奈米線稱為錐狀，經由PL、XRD、EDX都在在證明這些奈米線的品質是相當良好的。我們也成功的完成4軸對稱的氧化鋅陣列，控制成長的氧化鋅奈米線基本實驗奈米技術的一環，我們藉由介面的成功控制所想要的奈米線方線，而且不需要任何的催化劑或模版，只藉由TiN (100)的介面便可以完成。一個新的簡單成長垂直氧化鋅奈米線於TiN(111)的基板上，仍然不需要任何的催化劑，利用緩衝層的晶格結構與氧化鋅相似即可完成，而這兩種不同材料的晶格常數是相當相似，因此構成生長條件。

　　高密度單晶垂直的鋁參雜氧化鋅奈米線被製造出來，其鋁含量約為1.05 atom %，試片是在550°C於ZnO:Ga/glass基板上生長，其晶格常數也因鋁的參雜而增加約0.25%，光學特性也因而改變，電子場發射的能力也因此大幅的增加，由16 V/μm變成10 V/μm的良好特性，並由此推論其功函數由5.3eV下降到3.39eV。

　　採用高濃度的鎵加入合成氧化新奈米線時，觀察這合成的第二種現象的出現於垂直的氧化鋅奈米線上，其合成溫度為600˚C於ZnO/glass基板上，當鎵增加時，奈米線的長度因而減少，而X-ray有出現第二個材料的特性ZnGa2O4，也就是說，當鎵濃度僅僅為3.5 at. %，就會出現這第二個材料的物理特性，這說明氧化鋅不易出現高濃度的鎵參雜奈米線。高密度的氧化鋅與鋅鎵氧的core-shell結構，在600°C時合成於ZnO/glass基板上，X-ray可以很明顯的發現這兩種材料的峰值，而PL的結果也顯露出ZnGa2O4的對於PL的強度有很大幫助，但峰值卻也因此偏移到481 nm的位置。

　　垂直排列整齊之磷參雜之氧化鋅奈米線，採用蒸發反應的方式，在550°C被合成於ZnO:Ga/glass基板上，經驗證磷參雜之氧化鋅奈米線為單晶結構würtzite，方向是向著c軸的方向，磷參雜的影響的奈米線的長度，但不影響其直徑，而且也改變的其PL現象。

　Vertical single crystal ZnO nanowires with uniform diameter and uniform length were selectively grown on ZnO:Ga/glass templates at 600°C by self-catalyzed vapor-liquid-solid (VLS) process without any metal catalyst. It was found that the ZnO nanowires are grown preferred oriented in the (002) direction with a small x-ray diffraction (XRD) full-width-half-maximum (FWHM). Photoluminescence (PL), field emission scanning electron microscopy (FESEM) and high resolution transmission electron microscopy (HRTEM) measurements also confirmed good crystal quality of our ZnO nanowires. Field emitters using these ZnO nanowires were also fabricated. It was found that threshold field of the fabricated field emitters was 14 V/μm. With an applied electric field of 24 V/μm, it was found the emission current density was around 0.1 mA/cm2.

　Vertical single-crystal ZnO nanowires of were grown on ZnO:Ga/glass template by self-catalyzed vapor-liquid-solid (VLS) process at a low temperature of 520°C. It was found that length of these ZnO nanowires was around 2.0 μm while the diameter of these nanowires was in between 70 and 150 nm. It was also found that the ZnO nanowires were structurally uniform, defect free and well oriented with pure wurtzite structure. UV photodetectors were then fabricated using a simple scheme. It was found that photocurrent to dark current contrast ratio of our ZnO nanowires photodetector was 67.5.

　High density vertical single crystal ZnO nanowires were selectively grown on ZnO:Ga/Si3N4/SiO2/Si templates at various temperatures by two-step oxygen injection process of self-catalyzed vapor-liquid-solid (VLS) technology. It was found that tips of the ZnO nanowires are hexagon. It was also found that average length of the ZnO nanowires increased while average tip diameter of the ZnO nanowires decreased as the growth temperature increased. Furthermore, it was found that the ZnO nanowires grown at 500°C were “tube-shaped” while the ZnO nanowires grown at 700°C were “cone-shaped”. Photoluminescence (PL), x-ray diffraction (XRD) and energy depersive x-ray (EDX) results all indicate the quality of our ZnO nanowires is good.

　　This work reports an approach to preparing well-ordered, 4-fold symmetric ZnO nanowires arrays. Controlling the growth of nanowires is fundamental to realizing the dream of nanotechnology. The characteristics of the interface can be used to fabricate extended and oriented nanowires. As well as using a catalyst or template, a suitable buffer layer can be chosen to facilitate the control of the productive process, even though the crystal structure of the TiN (100) thus obtained differed entirely from that of ZnO in this study.

　A new and simple means of growing vertical ZnO NW arrays from the surface of a substrate using a TiN (111) buffer layer, but without using any catalysis or template, was proposed, although the crystal structure thus obtained differed entirely from that of ZnO. Using buffer layers, which have an appropriate lattice mismatch to the crystal of deposits, will induce island growth. Furthermore, epitaxial nanowire can be grown under the anisotropic growth condition.

　High-density, single-crystal, vertically-aligned, Al-doped ZnO nanowires with an Al content of 1.05 atom % were synthesized on ZnO:Ga/glass templates at 550°C. Although introducing Al did not change the physical dimensions of the ZnO nanowires, the lattice constant increased by 0.25% and the optical properties of the ZnO nanowires were degraded. However, the experimental results also showed that the threshold emission field can be significantly decreased from 16 to 10 V/μm, and the work function, can also be reduced from 5.3 to 3.39 eV by introducing Al atoms into the ZnO nanowires.

　This investigation describes the synthesis and the formation of the second phase of high-density arrays of vertically aligned ZnO:Ga nanowires on ZnO/glass substrates at 600˚C. As the concentration of the Ga is increased, the nanowire became shorter without any change in its diameter. The formation of the second phase, ZnGa2O4 (JCPDS No. 38-1240), was verified by X-ray diffraction even though the concentration of the Ga was only 3.5 at. %. The formation of the second compound substantially influenced the physical properties of the nanowire.

　High-density vertically aligned ZnO/ZnGa2O4 core-shell nanorods were synthesized on ZnO/glass templates at 600°C by reactive evaporation. X-ray diffraction (XRD) spectra revealed the composition of the sample. The core-shell structure was observed by energy-dispersive X-ray spectroscopic (EDX) mapping. The photoluminescence (PL) spectrum exhibited a strong peak at around 481 nm and a very high luminescent intensity.

　Vertically well aligned P-doped ZnO nanowires were prepared on ZnO:Ga/glass templates at 550°C by reactive evaporation without metal catalysts. The P-doped ZnO nanowires were found to be single crystal with a würtzite structure, oriented in the c-axis direction. P doping shortened the physical lengths of the ZnO nanowires without changing their diameter. Furthermore, the introduction of P atoms resulted in a much weaker and broader ZnO band edge emission.

CHAPTER 1 Introduction 18
1-1. The Background of Nanotechnology 18
1-2. Intrduction to one dimension nanomaterials 20
CHAPTER 2 ZnO nanowires synthetize methods and analyze equipments introduction 33
2-1. Various ZnO nanowires synthetize methods 33
2-1-1. Chemical Vapor Deposition method 33
2-1-2. Template-assisted growth method 34
2-1-3. Solution-base synthesis method 34
2-1-4. Catalyst-driven molecular-beam-epitaxy method 35
2-1-5. Metalorganic Chemical Vapor Deposition method 35
2-1-6. Vapor-Liquid-Solid (VLS) method 35
2-1-7. Self-catalyzed VLS process 36
2-2. Experimental details and analyze equipments introduction 37
2-2-1. Field-Emission Scanning Electron Sicroscope 38
2-2-2. High resultion X-ray diffractometer 39
2-2-3. FEI DualBeam System DB-235 39
2-2-4. Field Emission transmission electron microscopy 40
2-2-5. Photoluminescence Spectroscopy 40
CHAPTER 3 Single crystal ZnO nanowires grown on ZnO:Ga/galss and ZnO:Ga/Si3N4/SiO2/Si substrate 44
3-1. Vertical single crystal ZnO nanowires grown on ZnO:Ga/glass templates 44
3-2. Ultraviolet photodetectors with low temperature synthesized vertical ZnO nanowires 48
3-3. Selective growth of vertical ZnO nanowires on ZnO:Ga/Si3N4/SiO2/Si templates 51
3-4. Summarizes 54
CHAPTER 4 Epitaxial growth ZnO nanowire on TiN/Si Substrate 74
4-1. A New and Simple Means for Self-Assembled Nanostructure: Facilitated by Buffer Layer 74
4-2. Buffer facilitated epitaxial growth of ZnO nanowire 77
4-3. Summary 79
CHAPTER 5 Phosphorous, Aluminum and Gallium and doped ZnO nanowires synthesized on ZnO:Ga/glass templates 98
5-1. Vertically well aligned P-doped ZnO nanowires synthesized on ZnO:Ga/glass templates 98
5-2. Well aligned vertically Al-doped ZnO nanowires synthesized on ZnO:Ga/glass templates 101
5-3. Influence of the Formation of the Second Phase in ZnO:Ga Core-Shell Nanowire System 106
5-4. Summary 108
CHAPTER 6 Conclusion 130
Publication list 132

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Chapter 4
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Chapter 5
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