有序金屬奈米管陣列：菱形奈米管之表面增強拉曼散射與疏冰表面特性之研究

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研究生：	張庭豪 Ting-Hao Chang
論文名稱：	有序金屬奈米管陣列：菱形奈米管之表面增強拉曼散射與疏冰表面特性之研究 Rhombus mtallic nanotube arrays: Geometric effects on SERS and icephobic properties
指導教授：	朱瑾 Jinn P. Chu
口試委員:	姚栢文 Pak-Man Yiu 江偉宏 Wei-Hung Chiang 林宗宏 Zong-Hong Lin
學位類別：	碩士 Master
系所名稱：	工程學院 - 材料科學與工程系 Department of Materials Science and Engineering
論文出版年：	2023
畢業學年度：	111
語文別：	英文
論文頁數：	174
中文關鍵詞：	金屬奈米管陣列、表面增強拉曼、羅丹明6G 、結晶紫、葉酸、孔雀石綠、甲基巴拉松、萊克多巴胺、抗霜凍
外文關鍵詞：	Metallic Nanotube Array, SERS, Rhodamine 6G, Crystal violet, Folic acid, Malachite green, Methylparanate, Ractopamine, Anti-icing
相關次數：	點閱：350 下載：10
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在這項研究中，我們開發了一種金屬菱形奈米管陣列（MeNTAs）的製程技術，以達到高密度、有序的表面增強拉曼散射（SERS）應用與抗霜凍應用。這些菱形幾何形狀的MeNTAs具有緊密的間距。在實驗前期，我們使用有限差分時域（FDTD）模擬和實驗方法相結合，設計並製造了這些菱形MeNTAs。菱形MeNTA擁有大量的表面積，能夠吸附探針分子。在每平方公分面積上，奈米管的數量超過1億顆，且它具有可以產生SERS增強效應的熱點結構。
在這項研究中，我們首次提出了一種簡單且低成本的技術，使用DUV KrF微影製程和濺鍍過程在室溫下製造1x1 cm的MeNTA。掃描電子顯微鏡圖像顯示，菱形MeNTA基板具有高度有序的周期結構。我們進一步觀察到，菱形MeNTAs展現出優越的SERS效應。我們分別對羅丹明6G、結晶紫、葉酸、孔雀石綠、甲基巴拉松和萊克多巴胺等六種待測物分子進行測試，結果證明了菱形MeNTAs優異的性能。
此外，我們探討了菱形MeNTAs的潤濕性和抗霜凍能力。透過高速攝影機影像觀察水滴在菱形MeNTA基板上的撞擊形態，我們發現菱形MeNTA基板具有特別的潤濕性和抗霜凍能力。在抗霜凍實驗中，我們與先前實驗的光滑注液多孔表面(SLIPS)進行比較，菱形MeNTA基板，展現出良好的再現性與抗霜凍相關性能，反觀 SLIPS MeNTA有油膜，會隨著推冰柱循環量測次數的增加而降低性能表現。

This study reports novel rhombus metallic nanotube arrays (MeNTAs) for Surface-Enhanced Raman Scattering (SERS) and anti-icing applications. These rhombus MeNTAs possess closely packed nanotube arrays. First, we used Finite Difference Time Domain (FDTD) simulations with experimental techniques to design and fabricate these rhombus MeNTAs. There are over one hundred million rhombus nanotubes per cm2, which is thus potentially useful for SERS application.
This study introduces a simple and cost-effective method to produce 1x1 cm MeNTAs at room temperature, utilizing DUV KrF lithography and sputtering. Scanning electron microscopy images reveal that rhombus MeNTA substrates possess a highly ordered periodic structure. Furthermore, rhombus MeNTAs demonstrate superior SERS effects on six analytes, including Rhodamine 6G, Crystal Violet, Folic Acid, Malachite Green, Methyl Parathion, and Ractopamine. This confirmed the performance of the rhombus MeNTAs.
Finally, we investigated the wetting properties and anti-frosting capability of the rhombus MeNTAs. Using a high-speed camera, we observed the impact behavior of water droplets on rhombus MeNTA substrates and discovered their unique wetting properties and anti-frosting abilities. When compared to Smooth Liquid-Infused Porous Surface (SLIPS), SLIPS MeNTAs performed less well due to an increase in anti-icing cycles. In contrast, rhombus MeNTA substrates demonstrated reproducibility and correlation with anti-frosting properties.

摘要    I
Abstract    II
Acknowledgements    I
Content    II
List of Figures    V
List of Tables    XI
Chapter 1 Introduction    1
1    Objectives of study    2
Chapter 2 Literature Review    3
1 Metallic glass (MG)    3
1.2 Thin-film metallic glass (TFMG)    3
2 DUV KrF lithography (248nm)    5
3 Physical vapor deposition (PVD)    6
3.1 Step coverage    7
4 Metallic nanotube arrays (MeNTAs)    7
4.1 Fabrication of MeNTAs    7
4.2 Application of MeNTAs    13
4.2.1 MeNTAs as a SERS Substrate    13
5 The Finite-Difference Time-Domain (FDTD)    18
6 Plasmonics    19
6.1 Surface plasmon resonance (SPR)    19
6.2 Localized surface plasmon resonance (LSPR)    20
7 Surface-Enhanced Raman Scattering (SERS)    22
7.1 Electromagnetic enhancement (EM)    25
7.2 Chemical Mechanism (CM)    26
8 Potential application of Rhodamine 6G    27
9 Potential application of Crystal Violet (CV)    28
10 Potential application of Folic acid (FA)    30
11 Potential application of Malachite green (MG)    32
12 Potential application of Parathion methyl (PM)    33
13 Potential Application of Ractopamine    36
14 Superhydrophobic surface (SHS)    38
14.1 Surface wettability    39
14.2 Contact angle hysteresis (CAH)    44
15 Surface Icing Mechanisms and Theory    46
15.1 Icing mechanisms    46
15.2 Anti-icing    47
15.3 Ice adhesion (τ)    49
15.3.1 Observation of intrinsic ice adhesion versus macroscopic adhesion of ice    52
Chapter 3 Experimental Procedure    53
1 Fabrication of Rhombus Metallic Nanotube arrays (R-MeNTAs)    53
1.1 FDTD simulation    54
1.2 Photomask design    55
1.3 Substrate and photoresist preparations    56
1.4 Metallic thin film deposition    58
1.5 Photoresist removal    59
2 Characterization of metallic thin films    60
2.1 Scanning electron microscope (SEM)    60
2.2 Crystallographic analysis (XRD)    61
2.3 Wettability analysis    62
2.4 Surface roughness analysis (AFM)    63
2.5 Elemental surface analysis (AES)    64
3 Raman spectroscopy    64
3.1 Photomask design    66
3.2 Substrate and photoresist preparations    66
3.3 Adsorption of Rhodamine 6G onto R-MeNTA    66
3.4 Adsorption of Crystal Violet onto R-MeNTA    67
3.5 Adsorption of Folic acid onto R-MeNTA    67
3.6 Adsorption of Malachite green onto R-MeNTA    67
3.7 Adsorption of Parathion methyl onto R-MeNTA    68
3.8 Adsorption of Ractopamine onto R-MeNTA    68
4 Handheld Optical Power and Energy Meter    69
5 Superhydrophobic surface application    70
5.1 Mechanical Properties of Ice Formation (High-speed Camera)    71
5.2 Mechanical Properties of Adhesion and Shedding (Force Probe)    73
Chapter 4 Results and Discussion    74
1 Fabrication of Rhombus Metallic Nanotube arrays (R-MeNTAs)    74
1.1 FDTD simulation of Ag MeNTA with different geometry    74
1.1 Surface morphology (SEM)    76
1.2 Chemical composition analysis (EDS) of Ag R-MeNTA    77
1.3 Chemical composition analysis (AES) of Ag R-MeNTA    78
1.4 Crystallographic analysis (XRD)    80
1.5 Surface roughness analysis (AFM)    81
2 Raman spectra    83
2.1 Raman spectra of different geometries    84
2.2 Raman spectra of different polarization directions    85
2.3 Raman spectra Rhodamine 6G (R6G)    87
2.3.1 Raman spectra Rhodamine 6G (R6G) Limit of detection (LOD)    87
2.3.2 Raman spectra Rhodamine 6G (R6G) reproducibility    91
2.3.3 Raman spectra Rhodamine 6G (R6G) Raman mapping    92
2.4 Raman spectra Crystal Violet (CV)    95
2.4.1 Raman spectra Crystal Violet (CV) Limit of detection (LOD)    95
2.4.2 Raman spectra Crystal Violet (CV) reproducibility    99
2.5 Raman spectra Folic acid (FA)    100
2.5.1 Raman spectra Folic acid (FA) Limit of detection (LOD)    100
2.6 Raman spectra Malachite green (MG)    102
2.6.1 Raman spectra Malachite green (MG) Limit of detection (LOD)    102
2.7 Raman spectra Parathion methyl (PM)    104
2.7.1 Raman spectra Parathion methyl (PM) Limit of detection (LOD)    104
2.8 Raman spectra Ractopamine (RAC)    106
2.9 SEM images of different geometries before and after adsorption at the same concentration of R6G 10-4 M    108
3 Superhydrophobic surface application    111
3.1 Surface Morphology (SEM)    111
3.2 Wettability (Water contact angle)    114
3.3 Mechanical Properties of Ice Formation (High-speed Camera)    120
3.4 Mechanical Properties of Adhesion and Shedding (Force Probe)    130
3.5 Replace the MeNTA substrate with glass    134
Chapter 5 Summaries and Suggestions for Future Works    136
References    139
Appendix    152


                                

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