||Fabrication of Polymeric and Plasmonic Patterns on Flexible Substrate Based on Nanoimprint Lithography and Its Application to Superhydrophobic Surface and Refractive-Index Sensor
||Department of Photonics
Surface plasmon resonance
Refractive index sensing
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.
LIST OF TABLES XII
LIST OF FIGURES XIV
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)  63
3.3.2 Mie analysis  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
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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