臺灣博碩士論文加值系統

近年來，由電漿子金屬和不同的介電層半導體材料所組成的複合奈米結構因其特別而引人注目的表面電漿性質越來越受到重視。近期研究也指出藉由引入電漿子金屬產生電漿子強化光吸收效應和電漿子敏化現象，半導體材料的光催化效率也能因而提升。
在本博士論文中，我們合成了六角緊密堆積的金-二氧化鈦複合奈米陣列結構並進行光催化分解產氫的研究。透過結合膠體微影術、高溫熱退火處理、原子層沉積等技術，開發出了一套製程能成功的合成出大面積的六角緊密堆積的金-二氧化鈦複合奈米陣列結構，同時具有高度的陣列性跟均勻性。為了進一步探討其結構的表面電漿共振特性，量測了金-二氧化鈦複合奈米陣列結構的散射光譜，並透過理論模擬比照。在高反射率的二氧化鈦包覆的情況下，其表面電漿子共振波長呈現紅移，並且有分峰的情況出現，和理論模擬結果相符。
而在探討光催化分解產氫的實驗上，利用金-二氧化鈦複合奈米陣列結構做為催化物，無論是在可見光波段或是紫外光上，都有顯著的效率提升。透過時域有限差分法模擬可進一步看出在陣列結構上出現了電漿子引發局部強場的耦合，這說明了光催化效率提升的原因。同時不規則排列的金-二氧化鈦複合結構呈現了較差的效果，也說明了陣列結構的重要性。透過本篇論文的研究，對於未來設計電漿子金屬-半導體複合結構應用時，能有更深一層了解並有望達到更大的增益作用。

In recent years, hybrid nanostructures consisted of plasmonic metals and different dielectric materials have attracted much attention for their intriguing plasmonic properties. Recent studies have also shown that by introducing plasmonic metals, the photocatalytic efficiency of semiconductor can improve via plasmon-enhanced light absorption and plasmonic sensitization.
In this thesis, excellent photocatalytic properties for hydrogen production have been demonstrated by utilizing the hexagonal close-packed Au/TiO2 hybrid nanocrystal arrays. By combining colloidal lithography, dewetting process driven by surface energy and atomic layer deposition, a large area of hexagonal close-packed Au/TiO2 hybrid nanocrystal arrays with 100-110 nm single crystalline Au core and 10-40 nm TiO2 shell are prepared with highly ordered periodicity and uniformity.
To explore the localized surface plasmon resonance (LSPR) properties of the Au/TiO2 hybrid nanocrystal arrays, the scattering spectra were measured and compared with the simulation by Mie theory. The LSPR wavelength was found to be red-shifting and splitting into two LSPR peaks, correlating exactly to the simulated results based on Mie theory.
Under both ultra-violet and visible light, significant increase in the hydrogen production from 20% methanol solution water splitting was achieved with the hybrid Au/TiO2 nanocrystal arrays in comparison with bare TiO2 thin film as well as the randomly distributed Au/TiO2 nanocrystals. From the finite difference time domain simulation, the significant increase in hydrogen production can be correlated to strong and optimum coupling of the enhanced electric field from LSPR in Au/TiO2 nanocrystal arrays. In addition to allowing more accurate measurement of plasmonic enhancement, the ordered nanostructures have been shown to be especially amenable to the systematic analysis of lateral coupling of plasmonically enhanced electric field. As a result, optimal structures with appropriate spacing of core-shell metal-dielectric nanocrystals, metal core size and dielectric shell thickness for maximum enhancement can be designed.

Abstract I
摘要 III
Acknowledgments IV
Contents VI
Chapter 1 Introduction 1
1.1 Plasmonic Properties of Nanomaterials 2
1.1.1 Overview 2
1.1.2 Localized Surface Plasmon Resonance and Applications 3
1.1.3 Surface Plasmon Polariton (SPP) and Applications 6
1.2 Plasmonic Materials 8
1.3 Plasmonic Metals/Dielectric Materials Hybrid Nanostructures 9
1.4 Surface Plasmon Resonance-Enhanced Photocatalysis 11
1.4.1 Photocatalytic Reactions 11
1.4.2 Photocatalytic Water Splitting 13
1.5 Mechanisms of Photocatalytic Plasmon Enhancement 15
1.6 Motivations and Outline 17
Chapter 2 Experimental Section 19
2.1 Experimental Flowchart 19
2.2 Experimental Procedures 19
2.2.1 Fabrication of Hexagonal Au Nanocrystal Arrays 20
2.2.2 Fabrication of Hexagonal Au/TiO2 Hybrid Nanocrystal Arrays 20
2.2.3 Measurement of LSPR Properties of Au/TiO2 Hybrid Nanocrystal Arrays 21
2.2.4 Measurement of Plasmon-Enhanced Photocatalytic Properties of Au/TiO2 Hybrid Nanocrystal Arrays 21
2.3 Experimental 22
2.3.1 Electron Beam Gun Evaporation (E-Gun Evaporation) 22
2.3.2 Furnace Setup 22
2.3.3 Atomic Layer Deposition (ALD) 23
2.3.4 Scanning Electron Microscopy (SEM) 24
2.3.5 Focused Ion Beam (FIB) 25
2.3.6 Transmission Electron Microscopy (TEM) 26
2.3.7 Light-Scattering Spectroscopy 27
2.3.8 Rapid Thermal Annealing (RTA) 27
2.3.9 Gas Chromatography 28
Chapter 3 Fabrication and LSPR Properties of Au/TiO2 Hybrid Nanocrystal Arrays 29
3.1 Introduction and Motivation 29
3.2 Fabrication of Hexagonal Au/TiO2 Hybrid Nanocrystal Arrays 31
3.3 Measurement and Simulation of Scattering Spectrum of Au/TiO2 Hybrid Nanocrystal Arrays 37
3.4 Conclusions 41
Chapter 4 Plasmon-Enhanced Photocatalytic Hydrogen Production on Au/TiO2 Hybrid Nanocrystal Arrays 42
4.1 Introduction and Motivation 42
4.2 Plasmon Enhanced Photocatalytic Water Splitting by Au/TiO2 Nanocrystal Arrays and FDTD Simulation 45
4.3 Investigation with the Periodicity of the Au/TiO2 Nanocrystal Arrays and Plasmon Enhanced Photocatalysis 53
4.4 Investigation with Size of the Plasmonic Metal in Au/TiO2 Nanocrystal Arrays and Plasmon Enhancement in Near-Field 55
4.5 Conclusions 59
Chapter 5 Summary and Conclusions 60
Chapter 6 Future Prospects 62
6.1 Fabrication of Au-SiO2-TiO2 Hybrid Nanocrystal Arrays 62
6.2 Plasmon Enhancement of Photocatalytic Hydrogen Production on Plasmonic metals/TiO2 Nanostructures: Au/Ag/Al 66
References 68

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