臺灣博碩士論文加值系統

在物聯網與工業4.0時代中，可撓式材料因為其強大應用潛力而引起廣泛地研究與開發，同時，隨著近年來穿戴式電子設備的需求快速增長，因此各種可能提升可撓式電子元件功能表現的替代方案也被積極探索與開發。另一方面，在過去二十年來，氧化物磊晶薄膜也因為被視為可取代矽基半導體的潛力材料之一，而持續被深入研究。因此，可撓式氧化物磊晶材料被提出，用以實現兼有可撓性與氧化物材料之高功能性。然而，因為缺乏適合的可撓式基板以及現今可撓晶圓的繁雜製程，可撓式氧化物磊晶材料的開發上已遇瓶頸，為突破此瓶頸，此論文中我們將利用雲母作為可撓式基板，開發兩種可撓式氧化物磊晶系統，並在此兩子題目中，展示彎曲調控電子傳輸特性與探討背後物理機制。
第一個子題中，我們將以「氧化鋅成長於白雲母上之透明異質磊晶系統」開發新穎透明彎曲感測器，並凸顯其優異的穩定性與靈敏度。此外，我們也透過各種量測分析去討論其巨大的電阻率改變特性與機制，包含：結構、電子傳輸、光學、應變與材料模擬，並得出：彎曲、應變、壓電位差、電荷累積與電阻率改變，這一連串結論。藉由此題目，我們為彎曲感測器開闢出嶄新的研究方向，並展現彎曲感測器在智慧感測元件中的潛力。第二個子題中，我們將聚焦在具有奈米柱狀結構於表面的「鐠鈣錳氧磊晶薄膜」於氟晶雲母上。透過結合特定奈米結構與氟晶雲母的可撓性，此系統在不同彎曲狀態下表現出優異的龐磁阻調控特性(~ 1000 %)，顯示其在未來可撓式磁阻元件中的應用價值。在這子題中，我們主要藉由結構鑑定、吸收光譜與磁電傳輸特性量測，詳細探討此系統中的電子結構及磁性相態的轉變與其誘發之磁阻調控特性。綜合以上的研究成果，兩個子題皆以可撓式氧化物磊晶材料系統演繹出彎曲控制電子傳輸特性，並且展示其在新一代可撓電子元件中的應用價值。

Flexible electronic materials attract people’s attentions and have been extensively developed for its potential applications in the era of Internet of Things (IoT) and Industry 4.0. As the rapidly arising requirement is coming from flexible devices, scientists are looking for alternative solutions to comprehensively enhance their performance. In the meanwhile, heteroepitaxial oxide thin film has been explored in the past two decades because of its abundant functionalities and great potential to replace silicon-based semiconductor materials. Thus, flexible oxide heteroepitaxy is proposed to achieve great flexibility and retain high performance of oxides. However, the lack of suitable flexible substrates and the complicated process of fabrication hinder its development. To overcome these bottlenecks, in this thesis, we introduce muscovite (mica) as a flexible substrate and develop two mica-based flexible oxide heteroepitaxial systems. In addition, outstanding manipulations of their electrical properties via mechanical bending are exhibited and the physical mechanisms are deeply investigated.
In the first topic, Giant Resistivity Change of Transparent ZnO/muscovite Heteroepitaxy, a transparent flex sensor based on the heteroepitaxy of ZnO/muscovite is developed with the superior stability and sensitivity. In addition, the mechanism of the giant resistive change is studied with the scope of structure, transport, optics, strain and simulation. This topic demonstrates an extraordinary concept in the field of flex sensor for the design and development of next-generation smart sensor devices. In the second topic, Mechanical Modulation of Colossal Magnetoresistance in Flexible Epitaxial Perovskite Manganite, a finely designed Pr0.5Ca0.5MnO3 thin film with nanocolumn structure is developed on a F-mica substrate. Via the combination, this system presents the outstandingly mechanical modulation of CMR ratio (~ 1000 %) showing the potential in future flexible magnetoresistive devices. Besides, the tests of bending radius dependent resistance were carried out in a normal environment and demonstrated the tunability of near 30 %, which can be regarded as the potential in mechanical sensor devices. The detailed transitions of electronic states and magnetic phases are included for discussions. Generally speaking, both topics not only explores a field of mechanically tunable electrical properties by such designed heteroepitaxially flexible structures, but demonstrates their potential for future flexible electronic applications.

摘 要 i
ABSTRACT iii
ACKNOWLEDGEMENT v
CONTENTS vi
LIST OF FIGURES ix
Chapter 1 INTRODUCTION 1
1.1 A New Platform of Soft Technology Based on Muscovite 1
1.1.1 2D Materials and vdW Epitaxy 2
1.1.2 Muscovite 4
1.1.3 Functional Oxides Materials on Muscovite 6
1.1.4 MICAtronics – The Development of Electronics Based on Mica 10
1.1.5 The Future of MICAtronics 13
1.2 The Basic Properties of Zinc Oxide 16
1.3 The Basic Properties of Ca doped PrMnO3 18
1.4 Primarily Fundamental Features 20
1.4.1 Piezoelectric effect 20
1.4.2 Piezoresistance 23
1.4.3 Magnetoresistance 25
1.4.4 Magnetism 27
Chapter 2 EXPERIMENTAL METHODS 30
2.1 Sample Fabrication 30
2.1.1 Pulsed Laser Deposition 30
2.1.2 Sputter Deposition 31
2.2 Structural Characterization 33
2.2.1 X-ray Diffraction 33
2.2.2 Transmission Electron Microscopy 36
2.2.3 Scanning Electron Microscopy 38
2.3 Morphology 40
2.3.1 Atomic Force Microscopy 40
2.4 Spectroscopy 44
2.4.1 X-ray Photoelectron Spectroscopy 44
2.4.2 Raman Spectroscopy 45
2.4.3 X-ray Absorption Spectroscopy 48
2.5 Physical Properties 50
2.5.1 Transport – Physical Property Measurement System 50
2.5.2 Magnetic Properties – Vibrating Sample Magnetometer 52
2.6 Bending Measurement 53
Chapter 3 GIANT RESISTIVITY CHANGE OF TRANSPARENT ZnO/MUSCOVITE HETEROEPITAXY 55
3.1 Abstract 55
3.2 Motivation 55
3.3 Experimental Section 58
3.4 Prediction of ZnO/muscovite 59
3.5 Results and Discussion 62
3.5.1 Structural Characterization 62
3.5.2 Giant Resistivity Change 65
3.5.3 Hypothesis of Mechanism and Confirmation 67
3.5.4 Application of Strain 71
3.5.5 Establishment of Bending Model 73
3.5.6 Spatial Resolution of Resistivity Change 76
3.6 Demonstration of Transparent Mica Flex Sensor 77
3.7 Conclusions 80
Chapter 4 MECHANICAL MODULATION OF COLOSSAL MAGNETORESISTANCE IN FLEXIBLE EPITAXIAL PEROVSKITE MANGANITE 82
4.1 Abstract 82
4.2 Motivation 83
4.3 Experimental Section 85
4.4 Results and Discussion 86
4.4.1 Structural Characterization 86
4.4.2 Certification of Chemical Components 90
4.4.3 Magneto-transport 93
4.4.4 Mechanical Modulation of Colossal Magnetoresistance 95
4.4.5 Magnetism 100
4.5 Conclusions 102
Chapter 5 SUMMARY 104
APPENDIX. ESTABLISHMENT OF DOUBLE 2D STRUCTURE - THE GROWTH OF LiCoO2 ON MICA 106
A 1. Introduction 106
A 2. Experimental Methods 107
A 3. Results and Discussion 108
A 3 .1. Structural Characterization 108
A 3.1.1. X-ray Diffraction Analysis 109
A 3.1.2. Transmission Electron Microscopy 110
A 3.1.3. Raman Spectroscopy 112
A 3 .2. RHEED and Morphology 113
A 3 .3. Certification of Chemical Components 116
A 3 .4. Photostriction Measurements 116
A 4. Conclusions 118
REFERENCES 120

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