近年來科學家們致力於奈米雷射的相關研究，期望有朝一日能實際應用在晶片級光電元件上。其中最不可或缺的即是表面電漿共振效應於奈米雷射的應用，然而由於金屬吸收能帶以及能量容易耗散的問題使得紫外光波段雷射仍充滿許多不確定。
因此本研究將呈現我們的成果：以氧化鋅奈米線為基底的表面電漿雷射，搭配高介電常數的氧化物。
本研究藉由氧化鋅奈米線及單晶鋁基板，並在中間加入一層高介電常數材料作為絕緣體以形成表面電漿雷射。我們使用化學氣相沈積法合成高品質的氧化鋅奈米線並作為增益介質放在使用分子束磊晶沉積的單晶鋁基板上，同時，我們使用電子束蒸鍍沈積高介電常數的絕緣層（氧化鎢、氧化鉬、氧化鉈）並將其置於氧化鋅奈米線及鋁基板中間形成半導體—絕緣體—金屬複合結構SIM。此結構演示了極低的雷射閥值，相較於先前的氧化鋅—氧化鋁—鋁有相當卓越的突破，原因在於高介電常數絕緣層將能量有效的侷限在亞波長範圍內。
本實驗演示了四種不同的高介電常數材料作為絕緣層時對雷射閥值帶來的影響，結果顯示高介電常數材料可以得到較低的雷射閥值，介電常數越高，雷射閥值越低，而雷射閥值同時也與介電層的厚度有關。本實驗顯示出選去特定材料作為介電層有助於增加電磁場的強度。此外，材料的結晶性和缺陷程度都會影響雷射閥值。

Plasmonic nano lasers have garnered considerable enthusiasm as a frontier issue during the last decade. Plasmonic nano lasers with their integration compatibility, paves the way for the eventual realization of on-chip optoelectronic applications. Surface plasmon polaritons are the main characteristic in plasmonic nano lasers that exceedingly focus in the deep-subwavelength regime. Nevertheless, low threshold operating conditions in the ultraviolet (UV) wavelength zone are still uncertain due to the metal absorption and surface plasmon scattering losses induced by the metal-dielectric interface roughness. Therefore, in this dissertation, we present our work on the development of ZnO nanowire-based surface plasmon polariton (SPP) nano lasers with semiconductor–insulator– metal hierarchical nanostructures, which allows various possibilities for SPP nano lasers. Moreover, high-k oxides have been widely utilized as gate dielectrics in advanced MOS devices due to their high dielectric constant presenting advantages such as reduced gate leakage and are regarded as prospective materials for the storage of information and communication, optical interconnects, and computing.
In this thesis, we demonstrated an SPP nano laser consisting of ZnO nanowires coupled with a single-crystalline aluminum (Al) film and high-k dielectric materials as insulating interlayer. High-quality ZnO nanowires grown via chemical vapor deposition process (CVD) were used as the gain media placed over single-crystalline Al film deposited via molecular beam epitaxy (MBE). Meanwhile, a high-k dielectric constant material-based interlayer films (WO3, MoO3 and Ta2O5) were deposited in the midst of the ZnO nanowires and Al film, via e-beam technique, to prevent the optical loss from dominating the metallic region and enhance the optical confinement. The semiconductor-insulator-metal (SIM) hybrid structured SPP laser demonstrated an ultra-low threshold laser operation. This threshold value was strongly influenced and lowered than that previously reported in similar ZnO/Al2O3/Al plasmonic lasers. Such suppression of the lasing threshold is attributed to the insulating layer, which mediated the strong energy confinement of the optical field in the subwavelength regime.
Furthermore, comprehensive investigations of the critical roles of high-k dielectric interlayers on the lasing thresholds of ZnO/high-k material/Al nano lasers for four different dielectric layers have been conducted. The results demonstrated that the high dielectric constant materials as the interlayers over epitaxially grown Al film consisting of high-quality ZnO nanowires construct superb low threshold SPP lasers. It has been found that the lasing threshold varies with increasing thickness and reduces while increasing the dielectric constant. The performances are compared with similarly fabricated nano lasers with Al2O3 and WO3 dielectric interlayers. The critical roles of dielectric constants of the dielectric interlayers on influencing the thresholds of lasing are elucidated. This investigation indicates that the selection of appropriate dielectric interlayer film enhances sustenance of the electromagnetic field energy at room temperature. In addition, the crystallinity and defects of the dielectric layers are also contributing factors in influencing the lasing thresholds.

Abstract ........................................................................................................................................ i
摘要 .............................................................................................................................................. iii
Acknowledgements ...................................................................................................................... v
List of Figures .............................................................................................................................. vii
List of Tables ............................................................................................................................... xiii
List of Acronyms and Abbreviations ........................................................................................... xiv
Table of Contents ....................................................................................................................... xvi
Chapter 1 Introduction ............................................................................................................ 1
1.1 Thesis Rationale .................................................................................................................... 1
1.2 Thesis Structure .................................................................................................................... 2
Chapter 2 Research Background ............................................................................................ 3
2.1 Introduction ........................................................................................................................... 3
2.2 Overview of Nanotechnology ................................................................................................ 3
2.3 One-dimensional Nanostructures ......................................................................................... 4
2.4 Fabrication Techniques of 1-D Nanostructures ..................................................................... 6
2.4.1. Vapor-Liquid-Solid (VLS) Growth Mechanism ..................................................................... 6
2.5. Nano Lasers and Plasmonics ................................................................................................. 8
2.5.1. Development of Plasmonic Systems ............................................................................ 12
2.5.2 Nano Laser Device Design Considerations .................................................................. 14
Chapter 3 Experimental Techniques ...................................................................................... 21
3.1 Introduction .......................................................................................................................... 21
3.2 Methodology Flowchart of SIM-Configured Device Fabrication .......................................... 21
3.3 Experimental Procedures ..................................................................................................... 22
3.3.1 Fabrication of ZnO NWs ............................................................................................... 22
3.3.2 Fabrication of Dielectric Layers by Electron-Beam Evaporation .................................. 25
3.3.3 Growth of Epitaxial Aluminum Film by Molecular Beam Epitaxy (MBE) ........................ 25
3.4 Fabrication of SIM Nano Laser ............................................................................................ 26
3.5 Characterization Techniques ............................................................................................... 27
3.5.1. Electron-Beam Evaporation (E-Gun Deposition) .......................................................... 27
3.5.2. X-Ray Diffractometry (XRD).......................................................................................... 28
3.5.3. X-Ray Photoelectron Spectroscopy (XPS) ................................................................... 30
3.5.4. Scanning Electron Microscopy (SEM) .......................................................................... 30
3.5.5. Transmission Electron Microscopy (TEM) .................................................................... 32
3.5.6. Atomic Force Microscopy (AFM)................................................................................... 34
3.5.7. Spectroscopic Ellipsometry (SE) .................................................................................. 35
3.5.8. Micro-Photoluminescence (µ-PL) Optical Measurement System ................................ 37
Chapter 4 ZnO NWs on SC- Al Film Coupled with an Insulating WO3 Interlayer Manifesting Low Threshold SPP Laser Operation ........................................................................................... 39
4.1 Motivation and Introduction ................................................................................................. 39
4.2 Morphological Characteristics of Epitaxial Aluminum Film .................................................. 41
4.3 Morphological and Structural Properties of ZnO NWs ........................................................ 42
4.4 Effects on the Optical Properties of ZnO Nano Lasers ....................................................... 44
4.4.1 ZnO Nano Lasers Performance with Native Oxide ....................................................... 44
4.2.2 ZnO Nano Lasers Performance with Varying Thickness of WO3 ................................. 46
4.5 Surface Characterization of Dielectric Films ....................................................................... 50
4.5.1 Surficial and Compositional Effects on WO3 Films ...................................................... 50
4.5.2 Ellipsometry Properties of WO3 Films with Varied Thickness ...................................... 52
4.6 Simulated Characteristics of ZnO Nano Laser with Different WO3 Film Thickness ............ 53
4.7 Conclusions ......................................................................................................................... 55
Chapter 5 Superb Low threshold SPP Laser Operation with Tailored Dielectric Interlayers of Varied Thickness ......................................................................................................................... 56
5.1 Motivation and Introduction ................................................................................................. 56
5.2 Characteristics of ZhDlA Hybrid Structure Nano Laser ………….............................………....… 58
5.2.1 Effects of MoO3 Thickness on the Optical Lasing Properties of ZhDlA Nano Laser ... 59
5.2.2 Simulated Characteristics of ZnO Nano Laser with Different MoO3 Film Thickness … 61
5.2.3 Surficial and Compositional Properties of MoO3 Films ………………….......................…… 62
5.2.4 Ellipsometry Properties of MoO3 Films with Varied Thickness …………………...........…… 64
5.2.5 Ta2O5 Thickness Effects on the Optical Properties of ZhDlA Nano Laser ………………. 66
5.2.6 Simulated Characteristics of ZnO Nano Laser with Ta2O5 Dielectric Interlayer Film .. 68
5.2.7 Morphological Characteristics of Ta2O5 Dielectric Interlayer Films …………………..……. 70
5.2.8 Ellipsometry Properties with Altered Thickness of Ta2O5 Dielectric Interlayer Films .. 72
5.3 Comparison on Lasing Performance for Different Dielectric Interlayers ………………………….. 73
5.3.1 Crystallinity of the Different Dielectric Interlayers …………………………………………........…. 76
5.4 Conclusions ……………………………………………………………………………………….............................. 78
Chapter 6 Summary and Conclusions …………………………………………….......................…………… 79
Chapter 7 Future Perspectives ……………………....……………………………………………………………….. 81
7.1 Lasing Performance Enhancement through Coupling Bi-dielectric Spacing Film …………….. 81
7.2 Interface Engineering of Bi-Dielectric Films ……………………………………..………………….........… 83
APPENDIX ................................................................................................................................... 86
References ……………………........................................…………………………………………………………………91

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