近年來，迅速發展的物聯網系統正在改變人們的日常生活，為了發展全新的應用並滿足更多的需求，開發擁有優異表現的可撓式智慧材料成為了重要的議題。複雜性氧化物由於擁有眾多優秀的特性表現，並擁有極佳的熱與化學穩定性，將有很大的機會應用於未來科技當中。塊材的氧化物材料展現出非常吸引人的特性，然而卻有難以製作的缺點並且無法與其他材料系統結合，並且不具有彎曲的特性。因此，開發氧化物磊晶薄膜系統成為當前最重要的議題。然而，目前為止沒有任何技術能於商用的可撓式基板上直接成長磊晶的複雜性氧化物系統。近來由於成長技術的精進以及對於凡得瓦磊晶的瞭解，許多的技術被用來開發可撓式氧化物異質磊晶系統。
在此論文中，為了製造出具有可撓性的氧化物異質磊晶系統，作者研究並開發凡得瓦磊晶氧化物薄膜系統於二維層狀基板上。相較於傳統磊晶擁有強大的應力存在於薄膜與基板之界面，由於氧化物材料與二維層狀基板間僅有微弱的凡得瓦力存在，基板箝制效應將變得微弱並可忽視，因此能製造出特性更加優秀之系統。此外，若將二維層狀基板經過適當的處理，此二維層狀基板將表現出可彎曲性，因此高品質的可撓式氧化物異質磊晶將能被製造出來，並且應用於軟性電子元件當中。本論文之結果希望能提供全新的思維，用於增強未來元件之功能性及設計出全新的應用。

Over the past decades, a quick rise of the Internet of Things is changing our daily life. Therefore, high performance flexible smart materials to fulfill new applications are highly in demand. Complex oxides can play an important role due to their intriguing functionalities and superior thermal and chemical stabilities. Bulk oxides exhibit charming functions, however, they are hard to be fabricated or combined with other materials, and also are rigid. Therefore, the development of oxide epitaxial thin films is necessary, nevertheless, no direct growth techniques of epitaxial complex oxides on commercially flexible substrates are available. Recently, due to the advancement of growth facilities and the rise of knowledge of van der Waals epitaxy, various techniques have been employed to acquire flexible oxide heteroepitaxy.
In this thesis, to further approach the oxide heteroepitaxy with flexibility, the author develop van der Waals epitaxial oxide thin film systems on 2D layered substrates. Due to only weak van der Waals force exist between complex oxides and layered materials, the substrate clamping effect will become impotent and ignorable, which is different from conventional epitaxial systems. In addition, with appropriate modulation, the 2D layered substrates can become flexible, therefore, high performance flexible oxide heteroepitaxy can be revealed and creating new applications. This dissertation is written to offer a new thought towards the enhancement of functionalities and advanced design of novel applications.

摘要 i
Abstract ii
致謝 iii
Table of content iv
List of Figures vii
Chpater 1 Introduction 1
1.1 Motivation 1
1.2 Dissertation Outline 3
Chapter 2 Background 4
2.1 Oxide Heteroepitaxy for Next-Generation Devices 4
2.1.1 Complex Oxide 4
2.1.2 Oxide Heteroepitaxy 5
2.2 Flexible Epitaxial Oxide Thin Films 7
2.2.1 Removal of Substrates 7
2.2.2 Transfer Techniques 10
2.2.3 Direct Growth 16
2.3 van der Waals Heteroepitaxy 19
2.3.1 Conventional Epitaxy 19
2.3.2 van der Waals Epitaxy 20
2.3.3 Muscovite Mica 24
Chapter 3 Experimental Methods 26
3.1 Sample Fabrication – Pulsed Laser Deposition 26
3.2 Structure Characterization 28
3.2.1 X-Ray Diffraction 28
3.2.2 Transmission Electron Microscopy 30
3.3 Techniques for Measuring Physical Properties 32
3.3.1 Atomic Force Microscopy 32
3.3.2 Piezoresponse Force Microscopy 35
3.3.3 Ferroelectric Test System 37
Chapter 4 van der Waals Epitaxy of Functional MoO2 Film on Mica for Flexible Electronics 39
4.1 Introduction and Motivation 40
4.2 Experimental Procedures 43
4.3 Results and Discussion 44
4.3.1 Growth of van der Waals epitaxial MoO2 44
4.3.2 Structural and Chemical analysis 46
4.3.3 Microstructure 49
4.3.4 Transport Measurements 51
4.3.5 Flexible MoO2 Heteroepitaxy 54
4.4 Conclusions 57
Chapter 5 van der Waals Epitaxy of Flexible and Transparent VO2 Film on Muscovite 58
5.1 Introduction 59
5.2 Experiment Methods 61
5.3 Results and Discussion 62
5.3.1 Structural Characterizations 62
5.3.2 Metal-Insulator Transition of VO2 67
5.3.3 Bending Test 70
5.4 Summary 72
Chapter 6 Transparent Anti-Radiative Ferroelectric Heterostructure Based on Flexible Oxide Heteroepitaxy 73
6.1 Introduction and Motivation 74
6.2 Experimental Procedures 77
6.3 Results and Discussion 79
6.3.1 79
Transparent and Fleixlbe Ferroelectric Heterostructure 79
6.3.2 Structural Analysis 82
6.3.3 Bending Measurement 86
6.3.4 Anti-Radiation Test 91
6.4 Conclusions 93
Chapter 7 94
Summary 94
References 95

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