臺灣博碩士論文加值系統

隨著科學技術的進步，近幾十年來正在開發各式各樣之電子產品，許多金屬氧化物半導體材料已經在這個方向上被探索和討論，以滿足工業過程之需求。在過去幾年裡，這些半導體材料以其優良之特性，逐漸給人們留下深刻印象，在商業電子元件領域佔有一席之地；此外，人們逐漸將注意力集中於結合新穎奈米結構之性質上，不僅可以應用於材料、光電子、磁學、力學等基礎理論研究，且在奈米元件應用也具有顯著潛力；其中，氧化鋅是一種有前瞻性之二六族n型奈米材料(直接能隙為3.37 eV)，在室溫下具有60 meV之激子結合能，與其他奈米材料相比，它擁有不同優越的導電性能，以及良好之化學和生物分子檢測性質。本論文主要內容是藉由射頻磁控濺鍍法成長氧化鋅薄膜作為晶種層，在低溫下以簡易之水熱法成長氧化鋅奈米結構，可應用於光電和電子元件領域，如紫外光檢測器、氣體感測器、場發射元件、奈米發電機等。
本論文的實驗部分如下：利用X光繞射分析儀探討奈米柱的結晶特性，並通過場發射掃描式電子顯微鏡和高解析場發射穿透式電子顯微鏡分析奈米柱的表面結構，以能量散射X射線譜儀和X射線光電子能譜儀測定氧化鋅元素組成特徵，藉由光激發螢光譜儀研究樣品之光學性能，利用Keithley 2410/2400儀器、個人電腦和半導體參數分析儀對元件的電特性進行測試。在這項工作中，我們將探討這些元件與氧化鋅材料結構之間的關係，本論文結果分為四個部分：
第一部分是紫外光檢測器之研究，採用低溫水溶液法在玻璃基板上成長銅或鎳摻雜氧化鋅之奈米結構。結果表示，以兩種不同的摻雜劑製備光檢測器，上升時間和恢復時間縮短，光靈敏度提升，其原因是：(1) 銅複合體對電子之捕獲和去捕獲快於氧分子之吸附和解吸；(2) 鎳元素有助於電洞載子形成。因此，提高元件之光響應；其中，以0.003 M銅摻雜和4 mM鎳摻雜濃度之氧化鋅奈米柱為最佳值。與純氧化鋅光檢測器相比，在偏壓3 V和波長380 nm紫外光照射下，兩種光檢測器元件之靈敏度分別為196.6和393.04。
在研究的第二部分，藉由水熱法與摻雜劑、直流磁控濺射系統處理過程，在玻璃表面成功地合成氧化鋅奈米柱，製備鈷摻雜和金奈米粒子吸附在氧化鋅奈米柱上之氣體感測器。根據結果：(1) 在乙醇環境中，利用5 mM鈷摻雜之感測器具有良好氣體特性，並具有卓越之氣體響應和快速上升/恢復時間，在100 ppm乙醇氣體濃度和300 °C工作溫度，氣體響應達到90.71%；此外，(2) 金奈米粒子修飾氧化鋅奈米柱氣體感測器也具有良好氣體性能，與其它氣體相比，當工作溫度為150 °C，且甲醇濃度為1000 ppm時，氣體響應達到62.65%。結果表明，鈷摻雜和吸附金奈米粒子能有效地改善氧化鋅感測器之氣體響應。
在文章的第三部分，利用化學浴沉積法和光化學合成法在基板上製備場發射元件，並將鈀奈米粒子吸附於氧化鋅奈米結構上，根據結果：(1) 純氧化鋅和鈀奈米粒子吸附氧化鋅奈米柱之平均長度分別為2.11和2.14 μm，純氧化鋅和鈀奈米粒子吸附氧化鋅樣品之起始電場為6.6 和 6.4 V/μm，而場效增強因子分別為2546和5947；另一方面，(2) 在紫外光環境下，鈀奈米粒子吸附氧化鋅樣品之起始電場和場效增強因子分別約為5.6 V/μm和9145。根據以上結果，吸附鈀奈米粒子和在紫外光照射下可以改善氧化鋅場發射特性。
最後，在研究的第四部分，以新穎之氧化銦錫刻蝕技術和低成本水溶液合成方法製備鎵摻雜氧化鋅奈米發電機，藉由超聲波振動作為驅動力，量測奈米發電機之發電特性，根據實驗數據：(1) 鎵摻雜氧化鋅元件之輸出功率隨蝕刻時間上升而降低，最佳蝕刻時間為15分鐘，具有最大功率輸出特性。與純氧化鋅奈米發電機相比，鎵摻雜氧化鋅奈米發電機具有顯著的電特性；此外，鎵摻雜氧化鋅奈米發電機在紫外光照射下的輸出電壓和電流分別為0.128 V和1.51 × 10−6 A，實驗結果表示，鎵摻雜劑與在紫外光照射下能提高奈米發電機之發電特性。

With scientific and technological progress, a wide range of electronic products is being developed in recent decades. Many metal oxide semiconductor (MOS) materials have been explored and discussed in this direction to meet industrial process requirements. In the past few years, these semiconductors have gradually impressed people with their good properties, which have become a place in the field of commercial electronic devices. In addition, people are gradually focused on combining the properties of novel nanostructures, which can not only be used in basic theoretical research on materials, optoelectronics, magnetisms, and mechanics, but also have great potential for application in nanodevices. Among them, zinc oxide (ZnO) is a promising II–VI group n-type nanomaterial (wide direct energy band-gap of 3.37 eV), and has large exciton binding energy of 60 meV at room temperature. Compared with other nanomaterials, it has a variety of superior conductive properties, excellent chemical characteristics, and biological molecular detection performances. The main content of this thesis is ZnO thin films grown by radio frequency (RF) magnetron sputtering as seed layers, and ZnO nanostructures grown by simple hydrothermal method at low temperature, which can be used in the optoelectronic and electronic device fields, such as ultraviolet (UV) photodetectors (PDs), gas sensors, field-emission (FE) devices, and nanogenerators (NGs).
The experimental sections in this dissertation are as follows: the crystalline characteristics of nanorods (NRs) were measured using X-ray diffraction (XRD) spectrum analyzer, and the surface morphologies with elements were analyzed through field-emission scanning electron microscope (FE-SEM) and high-resolution transmission electron microscope (HR-TEM). The content composition characteristics of ZnO were explored using energy dispersive X-ray (EDX) spectrometer and X-ray photoelectron spectroscopy (XPS) instrument. Photoluminescence (PL) spectra were used to examine the optical performances of samples. The electrical properties of devices were also checked via the Keithley 2410/2400 equipment with a personal computer and a semiconductor parameter analyzer. In this work, we will explore the relationship between these devices and ZnO material structures. This dissertation results are divided into four parts:
The first part is the investigation of UV PDs. Copper (Cu)- or nickel (Ni)-doped ZnO nanostructures were grown on glass substrates by low temperature aqueous solution method. The results show the rise and recovery times of PDs prepared by two different dopants were shortened and the optical sensitivities increased. The reasons are as follows: (1) the trapping and de-trapping of electrons by Cu-related complexes were faster than the adsorption and desorption of oxygen molecules, and (2) the Ni element contributes to the formation of hole carriers. Therefore, the photoresponses of the devices were improved. Among them, the 0.003 M Cu-doped and 4 mM Ni-doped ZnO NRs were the best. Compared with pure ZnO PD, the sensitivities of the two PDs at 3 V applied bias and under 380 nm UV illumination were 196.6 and 393.04, respectively.
In the second part of the study, ZnO NRs were successfully synthesized on glass surface by hydrothermal method with the dopant and direct current (DC) magnetron sputtering system. Gas sensors with doping of cobalt (Co) contents or adsorption of gold (Au) nanoparticles (NPs) on ZnO NRs were fabricated. According to the results: (1) the sensor with 5 mM Co dopant shows excellent gas characteristics, and has superior gas responses and rapid rise/recovery times in an ethanol (C2H5OH) environment. The gas response reaches 90.71% at 100 ppm ethanol gas concentration and 300 °C operating temperature. Additionally, (2) the ZnO NR gas sensor modified with Au NPs also displays good gas-sensing performance. Compared with other gases, when the working temperature was 150 °C and the concentration of methanol (CH3OH) was 1000 ppm, the gas response reaches 62.65%. As a result, it can be seen that the gas responses of the ZnO sensor were effectively improved by the Co-doping and adsorption of Au NP.
In the third part of the article, the FE emitters were prepared on the substrate by chemical bath deposition (CBD) and photochemical synthesis, which were then palladium (Pd) NPs-adsorbed on ZnO nanostructures. Based on the results: (1) the average lengths of pure ZnO and Pd NPs-adsorbed ZnO NRs were 2.11 and 2.14 μm, respectively. The turn-on fields of pure ZnO and Pd NPs-adsorbed ZnO samples were 6.6 and 6.4 V/μm, whereas the effective field enhancement factors were 2546 and 5947, respectively. On the other hand, (2) the turn-on field and effective field enhancement factor of Pd NPs-adsorbed ZnO samples in the UV light environment were about 5.6 V/μm and 9145, respectively. According to the above results, the adsorption of Pd NP and UV light irradiation can improve the FE characteristics of ZnO.
Finally, in the fourth part of the research, the gallium (Ga)-doped ZnO NGs were fabricated using novel indium tin oxide (ITO) etching technology and low cost aqueous solution synthesis method. The power generation characteristics of the NG were measured by ultrasonic wave vibration as the driving force. (1) The experimental data show that the output power of the Ga-doped ZnO device decreases with increased etching time, and the optimal etching time was 15 min for maximum power generation characteristics. The Ga-doped ZnO NGs show remarkable electrical performance compared with pure ZnO NGs. Furthermore, the output voltage and current of Ga-doped ZnO NG under UV light irradiation were approximately 0.128 V and 1.51 × 10−6 A, respectively. Based on the experimental results, the power generation property of the NG can be enhanced by Ga dopant and UV light illumination.

摘要……….i
Abstract……….iii
Acknowledgements……….vi
Contents……….viii
Table captions……….xi
Figure captions……….xii
Chapter 1 Background and motivation……….1
1–1 Nanotechnology materials……….1
1–2 Organization of dissertation……….3
Chapter 2 Introduction……….4
2–1 Structural characteristic and application of ZnO material……….4
2–2 Physical properties of ZnO……….8
2–3 Piezoelectric (PZ) properties of ZnO……….8
2–4 Chemical properties of ZnO……….9
2–5 Electrical properties of ZnO……….9
2–6 Optical properties of ZnO……….9
2–7 Mechanical properties of ZnO……….10
2–8 Thermal properties of ZnO……….10
2–9 Literature review on the preparation methods for ZnO structure……….11
2–9–1 (Vapor-liquid-solid, VLS)……….12
2–9–2 (Vapor-solid, VS)……….13
2–9–3 (Solution-liquid-solid, SLS)……….14
2–9–4 (Metal organic chemical vapor deposition, MOCVD)……….15
2–9–5 (Pulsed laser deposition, PLD)……….16
2–9–6 (Whisker-growth)……….17
2–9–7 (Anodic alumina oxides, AAO)……….18
2–9–8 (Electrodeposition, ED)……….19
2–9–9 (Sonochemical method)……….21
2–9–10 (Hydrothermal method)……….23
2–10 Basic theory for different devices……….25
2–10–1 Theory of UV PDs……….25
2–10–2 Theory of gas sensors……….30
2–10–3 Theory of FE emitters……….32
2–10–4 Theory of NGs……….34
Chapter 3 Experimental section……….37
3–1 Experimental process……….37
3–2 Experimental instruments……….38
3–2–1 Measurement system for UV PDs……….38
3–2–2 Measurement system for gas sensors……….39
3–2–3 Measurement system for FE emitters……….40
3–2–4 Measurement system for NGs……….41
3–2–5 Field-emission scanning electron microscope (FE-SEM)……….42
3–2–6 High-resolution transmission electron microscopy (HR-TEM)……….43
3–2–7 X-ray diffraction (XRD)……….44
3–2–8 Photoluminescence (PL) spectrum……….45
3–2–9 X-ray photoelectron spectroscopy (XPS)……….46
3–2–10 Radio frequency (RF) magnetron sputtering……….47
3–2–11 Electron beam (E-beam) evaporation……….48
3–2–12 Direct current (DC) magnetron sputtering ……….49
3–2–13 Responsivity system……….50
Chapter 4 UV-sensing properties based on ZnO NRs with Cu dopants or Ni dopants……….51
4–1 Fabrication and characterization of UV PDs with Cu-doped ZnO NR Arrays……….51
4–1–1 Introduction……….51
4–1–2 Device structure and fabrication……….52
4–1–3 Results and discussion……….53
4–1–4 Conclusion……….57
4–2 Fabrication and characterization of Ni-doped ZnO NR arrays for UV PD application……….67
4–2–1 Introduction……….67
4–2–2 Device structure and fabrication……….68
4–2–3 Results and discussion……….69
4–2–4 Conclusion……….72
Chapter 5 Gas-sensing characteristics based on ZnO NRs with Co dopants or adsorbed Au NPs……….83
5–1 Characteristics of gas sensors based on Co-doped ZnO NR Arrays……….83
5–1–1 Introduction……….83
5–1–2 Device structure and fabrication……….84
5–1–3 Results and discussion……….85
5–1–4 Conclusion……….92
5–2 Hydrothermal synthesis and improved methanol-sensing performance of ZnO NRs with adsorbed Au NPs……….103
5–2–1 Introduction……….103
5–2–2 Device structure and fabrication……….104
5–2–3 Results and discussion……….105
5–2–4 Conclusion……….108
Chapter 6 FE performances based on ZnO NRs decorated with Pd NPs by photochemical synthesis……….118
6–1 Characteristics of field emitters based on Pd-adsorbed ZnO nanostructures with photochemical method……….118
6–1–1 Introduction……….118
6–1–2 Device structure and fabrication……….119
6–1–3 Results and discussion……….120
6–1–4 Conclusion……….123
6–2 UV-enhanced FE properties of Pd-adsorbed ZnO NRs through photochemical synthesis process……….131
6–2–1 Introduction……….131
6–2–2 Device structure and fabrication……….132
6–2–3 Results and discussion……….133
6–2–4 Conclusion……….135
Chapter 7 UV-enhanced NG properties of Ga-doped ZnO NR arrays……….145
7–1 Enhanced NG performances of 1-D Ga-doped ZnO NR arrays under UV light illumination……….145
7–1–1 Introduction……….145
7–1–2 Device structure and fabrication……….146
7–1–3 Results and discussion……….148
7–1–4 Conclusion……….152
Chapter 8 Summary and Future work……….167
8–1 Conclusion……….167
8–2 Future work……….169
References……….170
Extended Abstract……….199

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