首先，在大分子量嵌段共聚合物PS-PMMA薄膜中，藉由自組裝的方式可以得到一維或者是三維的光子晶體。並且透過選擇性溶劑的退火製程，可以獲得短程有序的網狀結構，這些結構展現出反射可見光波段的光學性質且具備與角度無相關的特色──稱之為無序型光子晶體，並且擁有對於外界溶劑感知的溶致變色特性。有趣的是，我們可以透過與均聚物PS-PMMA/PS/PMMA三相混摻的方式得到較大尺度的微相分離結構以及反射波段紅移的結果。此外，利用不同的混摻比例可以調控此高分子薄膜具有有序或無序型光子晶體的特性。由於PMMA經紫外光曝曬後具可裂解的特性，我們可以藉由此方法得到具網狀微結構之多孔高分子模板，而此模板可用於後續的二氧化矽以及二氧化鈦之溶凝膠製程，也進一步地說明，藉由溶凝膠製程我們可以導入不同的介電常數材料於無序型光子晶體薄膜中。最後，我們結合了光學微影以及自組裝的技術，成功地得到光學圖案化之無序型光子晶體薄膜。此外，利用上述之溶凝膠製程，也可以進一步地製備有機、無機以及複合物材料於此圖案化無序型光子晶體薄膜。綜合以上結果，我們以創新的概念製備出具有可光學圖案化及可導入不同材料特性的有序或無序型光學薄膜，並且期許這些結果可用於許多實際的應用當中。

Control of thin film morphologies through self-assembly of high-Mw polystyrene-b-poly (methyl methacrylate) (PS-PMMA) block copolymers (BCPs) are carried out to generate one-dimensional (1-D) or three-dimensional (3-D) polymer-based photonic crystals (PCs). By exposing the as-spun BCP film into a PMMA selective solvent for annealing, short-range ordered network morphologies can be obtained, resulting in the angle-independent reflected bands of amorphous photonic crystals (APCs) in responsive to external solvents in visible wavelength, namely solvatochromism. Performing BCP/homopolymer blends makes red shifting of the stop-band gaps due to the increased microdomain thickness. Most interestingly, the fabrication of the angle-dependent PCs or angle-independent APCs can be successfully carried out using PS-PMMA/PS/PMMA ternary blends. Taking advantage of the degradable characteristic of the PMMA segment allows us to first generate porous polymeric templates after exposure to UV irradiation and thereby inorganic SiO2 or TiO2 network microstructures via subsequent sol-gel processes and calcination, materializing the thin film photonic reflectors with high reflectivity and tunable refractive index contrast. Finally, with the integration of the top-down (i.e., photolithography) and bottom-up (i.e., rapid self-assembly) methods, the photopatterned APC thin films with organic, inorganic and hybrid materials are materialized for the first time. As a result, this provides a novel concept to materialize the organic, inorganic and hybrid APC or PC reflectors with the capability of pattern design in visible wavelengths for practical applications.

論文審定書 i
誌謝 ii
摘要 iii
Abstract iv
Table of Contents vi
List of Tables ix
List of Figures x
Chapter 1. Introduction 1
1.1 Self-Assembly 1
1.2 Block Copolymer (BCP) Self-assembly 3
1.3 Photonic Crystals in Nature 7
1.3.1 Fabrication of Photonic Crystals from BCP self-assembly 9
1.3.2 Stimuli-Responded BCP Photonic Crystals 13
1.4 Control of Optical Reflectivity of BCP Photonic Crystals 16
1.5 Amorphous Photonic Crystals in Nature 20
1.5.1 Fabrication of Amorphous Photonic Crystals 21
1.6 Inorganic Replicates from Templating of Porous BCP 24
Chapter 2. Objectives 27
Chapter 3. Materials and Experimental Methods 28
3.1 Materials 28
3.2 Sample Preparation 29
3.2.1 Bulks Samples Preparation 29
3.2.2 Thin Film Samples Preparation 30
3.2.3 PS-PMMA/PS/PMMA Ternary Polymer Blends 30
3.2.4 Porous Polymeric Templates Preparation 31
3.2.5 Porous SiO2 Templates Preparation 31
3.2.6 Porous TiO2 Templates Preparation 31
3.3 Microstructural and Photonic Characterization 32
3.3.1 Transmission Electron Microscopy (TEM) 32
3.3.2 Scanning Electron Microscopy (SEM) 32
3.3.3 Reflectivity measurements 32
Chapter 4. Results and Discussion 34
4.1 Microphase Separation of High-Mw PS-PMMA BCPs in bulk 34
4.2 Characterization of PS-PMMA BCP Thin Films 35
4.2.1 Microphase Separation of the High-Mw PS-PMMA BCP in Thin Films 35
4.2.2 Optical Properties of PS-PMMA Thin Film Reflectors 38
4.3 Replication of Network Microstructures 44
4.3.1 Porous Polymeric Templates 44
4.3.2 Inorganic Network Microstructures by BCP Templating 45
4.3.3 Optical Properties of Amorphous Photonic Crystals 50
4.4 Self-Assembly of PS-PMMA/Homopolymers Blends 52
4.4.1 PS-PMMA/Homopolymer Blends in Bulk 53
4.4.2 PS-PMMA/PS/PMMA Ternary Blends in Thin Film 55
4.5 Inverted Porous Inorganic Materials by Templating from Ternary Blends 58
4.5.1 Porous Polymeric Templates 58
4.5.2 Optical Properties of Amorphous Photonic Crystals from Ternary Blends 60
4.5.3 Replication of Porous Microstructures by Inorganic Materials 63
4.6 Optical-Patterned Amorphous Photonic Crystal Thin Films 67
4.6.1 Solvatochromic Properties of Patterned APC Thin films 67
4.6.2 Replication of Patterned APC Thin Films 71
Chapter 5. Conclusions 73
Chapter 6. References 75

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