數十年來，電漿子(Plasmonics)領域被深入地討論與研究，並且已發展於各種應用。其中，金(Au)通常被用於可見光到近紅外波段的研究，而貴金屬(Au、Ag)也已逐漸被其他電漿子材料取代，例如氮化鈦(TiN)。氮化鈦因為具有耐火特性以及可見光到近紅外波段的寬譜可調(broad adjustable) 共振而引起了人們的關注，並且與金相比，單晶的氮化鈦在小於 550nm的波段有著更小的損耗。
在此論文中，探究了電漿子在可見光波段的替代材料。因為電漿子的行為和強度主要由材料的品質決定，所以低損耗是可以被實現的。為了強調這個事實，我們利用低損耗和可大規模製造的單晶耐火氮化鈦薄膜去探討其對於熱光伏(thermophotovoltaics)的應用並且研究 氮化鈦/氮化鎵熱載流子次頻帶異質結構(heterostructures)中的光電導模態，結果顯示單晶的氮化鈦具有獨特又良好的光學、電學性質。
首先，由於氮化鈦在可見光和近紅外波段良好的光學特性、高熔點、出色的機械硬度以及在惡劣環境中的耐久性，其做為耐火的電漿子材料正被開發，所以針對氮化鈦耐火的特性探討其對太陽能收集(solar energy harvesting)的應用。近期，氮化鈦電漿超穎表面(plasmonic metasurfaces)被提出作為光學的寬頻譜吸收器(broadband absorbers)
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和窄頻譜熱發射器(narrow-band thermal emitters)，此兩者在高效能的太陽能熱光伏中都很重要。
我們展示了利用氮電漿輔助式分子束磊晶 (MBE) 在c面藍寶石基板長出延(111)面的抗氧化氮化鈦薄膜並將其製成在可見光吸收 90% 的單層超穎表面寬頻譜吸收器。與傳統反應濺鍍方法製備出的氮氧化鈦 (TiOxNy) 薄膜相比，MBE 成長的無氧氮化鈦薄膜具有優良的電漿子性質，通過穿透式電子顯微鏡 (TEM)、X光光電子能譜儀(XPS)、X光繞射儀(XRD)和原子力顯微鏡(AFM)證實了濺鍍出的氮化鈦和分子束磊晶成長氮化鈦的光學特性。結果顯示使用濺鍍方法製備出的氮化鈦不如分子束磊晶成長氮化鈦那樣的純正:以850°C真空退火濺鍍的氮化鈦樣品並且使用太陽光模擬器模擬130太陽(suns)的環境照射6小時後，發現濺鍍的氮化鈦無法承受如此高溫的環境，而分子束磊晶成長氮化鈦的超穎表面則具有出色的熱穩定性和化學穩定性。
在第二個工作中，將高效能電漿子的熱電洞注入光電導的氮化鈦/P型氮化鎵的異質結構:光電和光激發熱載流子的異質結構對於互補式金氧半導體(CMOS)在相容性、高穩定性和最快暫態時間(fastest transient time)方面具有極大潛力，其中一個獨特的熱載子裝置由耐火的氮化鈦/氮化鎵/藍寶石基板結合而成。在光激發載流子的應用中，作為替代材料的氮化鈦所受到的關注比其他電漿子材料(金、銀、銅、鋁)少，其特性尚不清楚，這裡我們提供了由分子束磊晶成長出的單晶氮化鈦/P型氮化鎵/藍寶石基板、
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氮化鈦/N型氮化鎵/藍寶石基板兩種異質結構，以穿透式電子顯微鏡證實異質結構的接面處結晶性良好，再採用電子束微影製程的方式製造裝置。將熱電洞(氮化鈦/P型氮化鎵/藍寶石基板)和熱電子(氮化鈦/N型氮化鎵/藍寶石基板)的兩種裝置與用於可見光波段的光電檢測氮化鈦奈米狹縫裝置比較。在1.95 eV的共振波長下以氮化鈦/N型氮化鎵相比，因為氮化鈦/P型氮化鎵在金屬與半導體的界面擁有光電導模態，其光電流、響應度和外部量子效率 (external quantum efficiency, EQE) 高出4個數量級，也透過X光光電子能譜儀與量測電流-電壓曲線各別分析氮化鈦/ P型氮化鎵以及氮化鈦/ N型氮化鎵的肖特基能障高度(Schottky barrier height)，分別為1.2 eV與0.6 eV。因此，量測氮化鈦的功函數(work function)求得肖特基能障高度解釋了熱載流子光電探測器的相對優勢和限制。最後總結了在可見光波段使用P型半導體作為光電耐火熱載流子裝置和電漿子驅動式光催化系統的材料是很好的選擇。

Plasmonics has been known for decades and has been used in various applications, primarily using gold (Au) for visible to NIR range. These days noble metal (Au, Ag) has been replaced with alternative plasmonic material such as Titanium Nitride (TiN). Titanium nitride has attracted interest due to its refractory characteristics and broad adjustable resonance from visible to the near-infrared regime. Moreover, one of the additional advantages we have introduced is that single-crystalline TiN is less lossy at wavelengths less than 550nm when compared to gold. Therefore, in this thesis, we explored the alternative plasmonic materials for the entire visible regime. As we know, the plasmonic behavior and strength are majorly dependent on the quality of materials so that the low loss can accomplish. Keeping this fact in mind, we explored the single-crystalline TiN film due to low-loss and mass-scale fabrication for designing the refractory TiN used for the thermophotovoltaics applications and hot carrier sub-band photodetection through TiN/GaN heterostructures, reported single-crystalline TiN has unique and tremendous optical and electrical properties.
Firstly, we studied the refractory Titanium nitride for solar energy harvesting; however, due to its outstanding optical characteristics in the visible and near-infrared ranges, high melting temperature, excellent mechanical hardness, and durability against material deterioration in harsh environments, titanium nitride (TiN) is developing material for refractory Plasmonics. TiN plasmonic metasurfaces have recently been proposed as optical broadband absorbers and narrow-band thermal emitters, both of which are important in high-efficiency solar thermophotovoltaics. We show that a single-layer metasurface broadband absorber fabricated from an oxidation-resistant TiN(111) epitaxial film grown on c-plane sapphire by nitrogen-plasma-assisted molecular beam epitaxy (MBE) can absorb 90% of visible light. In comparison to titanium oxynitride (TiOxNy) films made by the traditional reactive sputtering method, the oxygen-free stoichiometric TiN film created by MBE has improved plasmonic properties. The optical properties of sputtered TiN and MBE TiN has been confirmed from transmission electron microscopy (TEM), x-ray photoelectron spectroscopy (XPS), x-ray diffraction (XRD), and atomic force microscopy (AFM), which demonstrated that sputtered TiN is not pure TiN as MBE TiN. Furthermore, vacuum annealing at 850 °C using a vacuum sputtering system and irradiation of solar simulator under 130 suns in the ambient environment for 6 hours. That shows the sputtered TiN can’t survive in a very high-temperature environment, whereas MBE-grown TiN metasurfaces have excellent thermal and chemical stability.
We used plasmonics efficient hot-hole injection at the photoconductive TiN/p-GaN heterostructure for the second study. Here optoelectronic and photoexcited hot carriers TiN/GaN heterostructure devices have the greatest potential for CMOS compatibility, high stability, and fastest transient time. One of the unique combinations for hot carrier devices is refractory TiN/GaN/Sapphire. Alternative TiN has received less attention than other plasmonic materials (aluminum, silver, copper, and gold) for photoexcited hot carrier applications, and its properties are unknown. We have MBE grown single-crystalline TiN/p-GaN/Sapphire and TiN/n-GaN/Sapphire heterostructures. The crystalline properties of MBE grown TiN are investigated from TEM analysis. TEM analysis of the heterostructures shows good crystallinity of the heterostructures at the interface. Afterward, we have fabricated the device by electron beam lithography process. We have compared the two types of devices with hot holes (TiN/p-GaN/Sapphire) and hot electrons (TiN/n-GaN/Sapphire) with plasmonic TiN nanosilts photodetection empowered across the visible regime. Due to the photoconductive mode of the metal-semiconductor interface, TiN/p-GaN has a four-order higher photocurrent, responsivity, and external quantum efficiency (EQE) compared to TiN/n-GaN at the resonance wavelength of 1.95 eV. The Schottky barrier height in TiN/p-GaN between the interface was determined via XPS analysis and Schottky barrier height in TiN/n-GaN by I-V curve from Keithley 4200
SCS. Measured Schottky barrier height for TiN/p-GaN and TiN/n-GaN is 1.2eV and 0.6eV respectively. Consequently, the work function of TiN measured the Schottky barrier height of the TiN/p-GaN and TiN/n- GaN to explain the relative benefits and constraints of these hot carrier photodetectors. We concluded that using a p-type semiconductor for hot-carrier in visible regimes is a good approach for optoelectronic refractory hot-carrier devices (space sciences) and plasmon-driven photocatalytic systems.

ABSTRACT ......................................................................................................... 2
摘要 ....................................................................................................................... 5
ACKNOWLEDGMENTS ................................................................................ 10
TABLE OF CONTENTS ................................................................................. 12
LIST OF FIGURE ............................................................................................ 15
LIST OF TABLE .............................................................................................. 23
1. Chapter 1 ............................................................................................... 24
Introduction ................................................................................................. 24
1.1 Thesis Organization ........................................................................... 26
2. Chapter 2 ............................................................................................... 27
Background .................................................................................................. 27
2.1 Losses in Conventional Plasmonic Materials .................................... 27
2.2 Refractory Plasmonic Materials ........................................................ 29
2.3 Surface Plasmon Polaritons ............................................................... 32
2.4 Refractory Materials as Perfect Absorber ......................................... 35
2.5 Plasmonic Hot-Carrier Photodetectors .............................................. 38
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3. Chapter 3 ............................................................................................... 43
Titanium Nitride as Alternative Plasmonic Materials ................................. 43
3.1 Introduction of Titanium Nitride ....................................................... 43
3.2 Molecular Beam Epitaxy Growth of Titanium Nitride on Different Substrate ....................................................................................................... 44
3.3 Growth of Sputtered Titanium Nitride .............................................. 46
3.4 Crystalline and Optical Properties of the MBE and Sputtered TiN .. 47
3.5 Electrical Properties of Epitaxial TiN Film ....................................... 50
3.6 Fabrication of Nanoholes array and Nanosilts .................................. 51
4 Chapter 4 ............................................................................................... 53
Titanium Nitride for Solar Energy Harvesting Applications ...................... 53
4.1 Introduction and Motivation .............................................................. 53
4.2 Optical properties of Sputtered and MBE TiN film .......................... 56
4.3 Growth Comparison of Sputtered and MBE TiN .............................. 58
4.4 Optical Measurements and Fabrication of Metasurfaces .................. 61
4.5 Comparison of Sputtered and MBE TiN Metasurfaces ..................... 66
4.6 Conclusion ......................................................................................... 71
5 Chapter 5 ............................................................................................... 72
Epitaxial TiN/GaN Heterostructure for Efficient Photonic Energy Harvesting ............................................................................................... 72
5.1 Introduction and motivation .............................................................. 72
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5.2 Growth of Heterostructure TiN/p-GaN and TiN/n-GaN ................... 75
5.3 Fabrication of Hot-carrier Device ...................................................... 78
5.4 Optical measurement of TiN/n-GaN and TiN/p-GaN ....................... 80
5.5 Band Diagram of TiN/n-GaN and TiN/p-GaN .................................. 82
5.6 Electrical measurements of Hot-carrier Devices ............................... 87
5.7 Conclusion ......................................................................................... 93
6 Chapter 6 ............................................................................................... 94
Summary ...................................................................................................... 94
BIBLIOGRAPHY ............................................................................................. 97
APPENDIX ...................................................................................................... 111

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