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系統識別號 U0026-2505201612334200
論文名稱(中文) 利用奈米壓印微影術在可撓式基板上製作高分子與金屬奈米結構應用於超疏水表面與折射率之感測
論文名稱(英文) Fabrication of Polymeric and Plasmonic Patterns on Flexible Substrate Based on Nanoimprint Lithography and Its Application to Superhydrophobic Surface and Refractive-Index Sensor
校院名稱 成功大學
系所名稱(中) 光電科學與工程學系
系所名稱(英) Department of Photonics
學年度 104
學期 2
出版年 105
研究生(中文) 梁家慶
研究生(英文) Chia-Ching Liang
學號 L78001208
學位類別 博士
語文別 英文
論文頁數 220頁
口試委員 口試委員-陳學禮
口試委員-李佳翰
口試委員-謝健
口試委員-鄭宗杰
召集委員-賴韋志
指導教授-林俊宏
中文關鍵字 奈米壓印微影術  軟式模具  可撓式基板  表面電漿共振  折射率感測  超疏水表面 
英文關鍵字 Nanoimprint lithography  Soft mold  Flexible substrate  Surface plasmon resonance  Refractive index sensing  Superhydrophobic surface 
學科別分類
中文摘要 近年來,因受到市場的需求,在光電、有機電子、生物科技領域發展出許多非傳統的應用,特別是應用在可撓式元件上得到很多科學家的關注,其包含了發光二極體、太陽能電池、能量儲存器、液晶顯示器、人工瞳孔、生醫感測器、奈米紙傳感器…等。在結構製作上,利用傳統光學微影和電子束微影製程在不易直接在可撓式非平坦表面之基板上製作出結構,因此使用奈米壓印之技術是一個較合適的方式。然而大部分的高分子基板,容易與光阻溶劑不相容且有較差的熱穩定性,因此不適合使用傳統複雜的積體電路製程來製作。基於此因素,可撓式元件在製作過程中因盡量避免多步驟的製程、蝕刻步驟和接觸到有機溶劑的機會,因此利用奈米壓印微影術會是一個較合適的製作方式,近年來也發產出許多利用奈米壓印製作出可撓式元件之新穎製程。在本篇論文,我們提出三種與奈米壓印相關簡單的製程,其皆可直接在可撓式基板上製作出高分子或金屬週期性結構。
第一種製程,我們利用全氟聚醚軟式模具直接在聚碳酸酯基板上製作出週期性結構,全氟聚醚軟式模具相較矽模具和聚二甲基矽氧烷模具能在較低溫及較低壓力的條件下製作出結構,我們進一步詳細探討其原因,最後利用八氟環丁烷氣體對聚碳酸酯結構蝕刻形成多層結構,並具有超疏水表表面之特性。第二種製程,我們利用聚二甲基矽氧烷軟式模具直皆對金奈米顆粒溶液壓印出金週期性結構,藉由觀察退火溫度和時間對於結構局部表面電漿特性的影響找出最佳的退火參數,最後將此金奈米結構應用在折射率之感測,局部表面電漿之共振波長可以藉由改變結構的大小從可見光範圍調整至紅外光範圍,因此提高很寬的感測範圍。第三種製程,我們利用奈米轉印之技術,在NOA63高分子薄膜上,製作出特殊的金奈米褶狀結構,金奈米褶狀結構有一個極小腔體其寬度相較於轉印之PFPE結構寬度有很大幅度的縮小,我們也詳細探討其縮小的機制。金奈米褶狀結構相較於過去常用之金奈米孔隙有更好的光學特性表現,最後亦將此結構應用折射率之感測,在相位訊號的感測上有很好的感測能力,感測之品質因素可以高達40.1。以上提出之製程皆具有快速、低成本、大面積和能夠大量製作之優點,對於在可撓式元件之應用是很不錯的選擇。
英文摘要 In recent years, an increasing number of nontraditional applications have been developed in the areas of photonics applications, organic electronics, and biotechnology. In particular, flexible device applications, which include electronic devices, light-emitting devices, solar cells, energy storage devices, optical devices, flexible displays, artificial iris, surface-enhanced Raman scattering, nanopaper transducers, biomedical devices, bioinspired materials, and sensors, have gained considerable interest from various fields. Compared with conventional lithography, such as photolithography and e-beam lithography, nanoimprint lithography (NIL) is a suitable method to imprint the resist directly on flexible substrates because it can mold the resist on a nonflat surface. However, flexible substrates cannot be integrated easily into conventional integrated circuit fabrication processes because of the incompatibility of photoresists, low thermal stability, and complex fabrication procedures. Multiple processes should be eliminated, and dry etching or solvent treatment should be avoided. Several researchers have introduced many approaches based on NIL. In this thesis, we demonstrate three straightforward and convenient processes, which can fabricate polymeric patterns or metallic nanostructure on a flexible substrate.
In the first section, we show a reliable process for the direct nanoimprinting of a flexible polycarbonate (PC) sheet using a perfluoropolyether (PFPE) mold. The imprint performance of PFPE, hard/soft- PDMS and silicon molds are compared. Only PFPE mold can be fully patterned into PC substrate with viable integrity at a low heating temperature and applying pressure. The mechanical property and gas permeability of the materials are investigated. Finally, nanoroughness-on-nanopillar hierarchical surfaces, which possess superhydrophobic slippery characteristics, are obtained by treating PC nanopillar arrays imprinted by PFPE mold with C4F8 plasma. In the second section, we demonstrated the plasmonic metallic nanostructure fabricated by direct nanoimprinting of gold nanoparticles (AuNPs). The localized surface plasmon resonance properties of AuNPs or gold pillar arrays can be controlled and tuned during the annealing process. We apply this gold pillar arrays to refractive index sensing. The corresponding resonance wavelengths can be widely tuned from the visible to infrared region by changing the size of the gold pillars, thus providing a broad range of sensing capability. In the third section, we present a novel process based on nanotransfer printing for fabricating gold nano-pleat arrays. The gold film deposited over nano-ridge arrays on a PFPE mold was transferred directly to an NOA63 film on a glass substrate. The width of the nanocavities on the nano-pleat array can be dramatically reduced compared with the width of the nanoridges on the mold. The mechanisms of remarkable reduction in the nanocavity width during the gold sputtering process were investigated. Plasmonic properties of nano-pleat arrays have been studied numerically and experimentally. A sharp phase dip was used for refractive index sensing, demonstrating an excellent sensitivity with a figure of merit of 40.1. Above proposed fabrication processes are very simple, low-cost and high throughput. Thus, these are promising candidates for flexible device fabrication.
論文目次 口試合格證明 I
摘要 II
ABSTRACT IV
誌謝 VI
CONTENT VIII
LIST OF TABLES XII
LIST OF FIGURES XIV
ABBREVIATION XXV
CHAPTER 1 INTRODUCTION 1
1.1 Background of the Research 1
1.2 Motivation 1
1.3 Organization of the Thesis 2
CHAPTER 2 LITERATURE REVIEW 5
2.1 Nanoimprint Lithography (NIL) 5
2.1.1 mold materials 6
2.1.2 resist materials for nanoimprinting 9
2.2 Fabrication of Metal Nanostructure 10
2.2.1 solution-phase syntheses 10
2.2.2 top-down (conventional) approach 11
2.2.3 unconventional approach 12
2.3 Nanostructured Plasmonic Sensors 13
2.3.1 propagating surface plasmon resonance 14
2.3.2 localized surface plasmon resonance 17
2.3.3 Fano resonance 21
CHAPTER 3 EXPERIMENTAL SECTION 61
3.1 Mold Fabrication 61
3.1.1 silicon mold 61
3.1.2 preparation of polymer molds 61
3.2 Contact Angle Measurement 62
3.3 Simulation Method 63
3.3.1 rigorous coupled-wave analysis (RCWA) [108] 63
3.3.2 Mie analysis [109] 63
3.4 Nanoimprint of Flexible Polycarbonate Sheet with Flexible Polymer Mold and Application to Superhydrophobic Surface (chapter 4) 63
3.4.1 fabrication of superhydrophobic surface 63
3.4.2 material characterization 64
3.5 Plasmonic Metallic Nanostructures by Direct Nanoimprinting of Gold Nanoparticles (chapter 5) 64
3.5.1 synthesis the AuNPs 65
3.5.2 direct nanoimprinting of AuNPs 65
3.5.3 characterization 66
3.6 Nanotransfer Printing of Plasmonic Nano-pleat Arrays with Ultra-Reduced Nanocavity Width Using Perfluoropolyether Molds (chapter 6) 66
3.6.1 fabrication of nano-pleat arrays 66
3.6.2 characterization 67
3.6.3 refractive index sensing 68
CHAPTER 4 NANOIMPRINT OF FLEXIBLE POLYCARBONATE SHEET WITH FLEXIBLE POLYMER MOLD AND APPLICATION TO SUPERHYDROPHOBIC SURFACE 72
4.1 Introduction 73
4.2 Results and Discussion 76
4.2.1 direct nanoimprinting of PC sheet 76
4.2.2 effects of imprinting conditions 77
4.2.3 relaxation modulus of PC 80
4.2.4 air-trapping the mold cavity 82
4.2.5 stretch of PC nanostructures 85
4.2.6 imprinted PC nanopillar array as a superhydrophobic surface 86
4.3 Summary 91
CHAPTER 5 PLASMONIC METALLIC NANOSTRUCTURES BY DIRECT NANOIMPRINTING OF GOLD NANOPARTICLES 109
5.1 Introduction 110
5.2 Results and Discussion 112
5.2.1 as-synthesized nanoparticles 112
5.2.2 imprinting temperature 112
5.2.3 imprinting pressure 113
5.2.4 optical response 114
5.2.5 refractive index sensing 115
5.2.6 annealing time effect 117
5.3 Summary 120
CHAPTER 6 NANOTRANSFER PRINTING OF PLASMONIC NANO-PLEAT ARRAYS WITH ULTRA-REDUCED NANOCAVITY WIDTH USING PERFLUOROPOLYETHER MOLDS 128
6.1 Introduction 129
6.2 Results 132
6.2.1 fabrication of freestanding gold nano-pleat arrays 132
6.2.2 mechanisms of the nanocavity width reduction 134
6.2.3 optical properties of the nano-pleat arrays 139
6.2.4 geometry effects of nano-pleat arrays 144
6.2.5 filled thickness effect 148
6.2.6 refractive index sensing 151
6.3 Summary 153
CHAPTER 7 CONCLUSION 178
7.1 Nanoimprint of Flexible Polycarbonate Sheet with Flexible Polymer Mold and Application to Superhydrophobic Surface 178
7.2 Plasmonic Metallic Nanostructures by Direct Nanoimprinting of Gold Nanoparticles 180
7.3 Nanotransfer Printing of Plasmonic Nano-pleat Arrays with Ultra-Reduced Nanocavity Width Using Perfluoropolyether Molds 181
7.4 Summary 182
7.5 Future Work 183
REFERENCE 185
PUBLICATION LIST 217
A. Journal Paper 217
B. Conference Paper 218
APPENDIX A BACK COVER IN ADVANCED MATERIALS INTERFACES JOURNAL 220
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