氧化銅上的石墨烯在快速化學氣相沉積過程中的成核以及成長動力學

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莊敏強(Min-Chiang Chuang) 查詢紙本館藏

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物理學系

論文名稱

氧化銅上的石墨烯在快速化學氣相沉積過程中的成核以及成長動力學
(Nucleation and growth kinetics of graphene growth on copper oxide substrate in a rapid thermal chemical vapor deposition process)

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摘要(中)

石墨烯是一種由碳原子組成的二維薄膜，其厚度僅有一層原子層厚。自從2004年 Geim和 Novoselov 用膠帶法從石墨中剝離出石墨烯後，使得石墨稀的研究有著飛躍性的成長。二維空間的限制使得石墨烯有著獨特的線性色散關係，使得石墨烯有高電子遷移率、高透光性、堅韌且富有可撓性。這些特性讓石磨烯有著豐富的應用潛力。然而，高品質的石墨烯在工業上難以大量製造，這也成了石墨烯應用的瓶頸。在眾多製造石墨烯的方法中，化學氣相沉積被認為是最有可能工業化的方法，其優點為容易大量製造且便宜。為了提升石墨烯在工業上的應用，有兩個重要的重要的關鍵：大量製造和提升石墨烯的品質。
化學氣相沉積的製造限制在於冗長的升溫及降溫時間，一種利用鹵素燈加熱的快速升溫系統可以大量節省製呈時間。然而用此方法生成的石墨烯單晶非常微小，僅有微米等級；另一方面，Rouff 的團隊利用氧化銅為基板可以成長出公分等級的石墨烯單晶，此方法大大提升了石磨烯的品質，可以達到近乎無缺陷的石墨烯。
我們的研究結合了上述兩種的方法來達成快速且高品質的石墨烯製程，其中，我們特別關心氧在化學氣相沉積中所扮演的角色以及動力學。我們利用JMAK模型來分析石墨烯成長的相變化，並且利用了凝態物理中常用的相關方程式來定量分析不同的化學氣相成長機制。

摘要(英)

Graphene is a two dimension thin film consisted with carbon atoms in honeycomb ordered. Due to its unique band structure, graphene as unique electronic and material properties. Therefore graphene is expected to have great application potential in the future. However, it is still challenging to produce large amount and perfect graphene which is suitable for the application. This shortage limited the ceiling of the potential of graphene. Among all possible solution to produce large amount and defect-free graphene, chemical vapor deposition seems like to be the possible way to fabricate industry scale graphene.
Three of the key issues in chemical vapor deposition is the time, cost and quality of graphene. First, nowadays it is the guarantee way to form large and perfect graphene in lower pressure chemical vapor deposition system. However, such a grain needs long growth time which is impossible to meet the needs of industry scale. Also, the long heating and cooling time for furnace decrease the throughput of graphene. Second, hot wall furnace waste unwanted heat into the environment which is not helpful for the chemical vapor deposition process. Third, the quality of graphene of CVD is comparing poorly with mechanical exfoliation. In order to suit above issues, rapid thermal chemical vapor deposition is considered.
Although rapid thermal chemical vapor deposition is a low cost and fast production way to grow graphene, the graphene grain is small due to the non-equilibrium heating process. Recently this issue is solved by growing graphene on copper oxide. By exposing the oxygen on the defect on copper, rapid thermal chemical vapor deposition is able to grow large single crystal graphene. However, the underlying mechanism is still the shortage.
In this work, we investigate the role of oxygen in graphene chemical vapor deposition on copper oxide. We find out the mechanism of the nucleation and growth process with oxygen exposure by extending the JMAK model into a non-equilibrium region to explain the initial situation of CVD process. The extending JMAK model is able to explain the increasing in nucleation rate. In addition, a correlation function analysis in traditional condensed matter physic is workable to quantify the spatial distribution and uniformity of Graphene Island. This analysis also points out the transition from carbon forming new grain at local nucleation site to joining larger cluster and coalescence after oxygen exposure.

關鍵字(中)

★ 石墨稀
★ 化學氣相沉積

關鍵字(英)

★ graphene
★ Chemical vapor deposition

論文目次

摘要 i
Abstract ii
致謝 iv
Content v
List of figures x
List of tables xxi
Chapter 1 Introduction 1
1.1 Introduction 1
1.2 Motivation 3
1.3 Thesis outline 5
Chapter 2 Background 6
2.1 Introduction to Graphene 6
2.1.1 Graphene history 7
2.1.2 The structure of graphene 8
2.1.3 Tight binding mode calculation on graphene 9
2.1.4 Graphene in relativistic frame work 13
2.1.5 Relativistic Schrodinger/Klein-Gordon equation 13
2.1.6 Dirac equation 15
2.1.7 Energy level in strong magnetic field 15
2.1.8 Quantum Hall effect 18
2.2 Graphene fabricates method 20
2.2.1 Mechanic exfoliation 20
2.2.2 Chemical Exfoliation 21
2.2.3 Graphene formation by SiC 23
2.3 Graphene application 25
2.3.1 Graphene FET 25
2.3.2 Sensors 26
2.3.3 Transparent conductive films 27
2.3.4 Graphene electrode and supercapacitors 28
2.4 Introduction to CVD graphene 29
2.4.1 CVD history and key progress 30
2.4.2 Brief description of CVD graphene setup 31
2.4.3 Thermodynamic of graphene 33
2.4.4 Nucleation and Growth of graphene films 34
2.4.5 The pretreatment of copper surface 40
2.4.6 The role of transition metal 41
2.4.7 Compare the Mechanism in Cu and Ni 43
2.4.8 The role of the flow 44
2.4.9 Rate limiting model 45
2.4.10 The fractal dimension and diffusion limit aggregation 47
2.4.10.1 Introduction to fractal dimension calculation 47
2.4.10.2 Box counting calculation 51
2.4.10.3 RTCVD 52
2.4.10.4 Oxidation treatment 53
2.5 Characteristic method on graphene 54
2.5.1 Raman Spectroscopy 55
2.5.1.1 Raman scattering 55
2.5.1.2 Raman spectroscopy on graphene 56
2.5.2 X-ray photoelectron spectroscopy (XPS) 60
2.5.3 Scanning electron microscopy 61
2.5.4 Atomic force microscopy 64
2.5.4.1 Working principle 64
2.5.4.2 Van der Waals force 64
2.5.4.3 Lennard-Jones potential 65
2.5.4.4 Contact mode 66
2.5.4.5 Tapping mode 68
2.5.5 JMAK model 71
Chapter 3 Experiment method 77
3.1 Rapid thermal chemical vapor deposition system 77
3.2 The CVD process 79
3.3 Graphene transfer method 81
3.4 Method and data analysis 82
3.4.1 Image processing by image J 82
3.4.2 Image process 83
3.4.3 Fractal dimension calculation 86
3.4.4 Calculation of correlation function 87
3.4.5 Local anodic oxidation. 88
Chapter 4 Result and discussion 90
4.1 Result on CVD graphene 90
4.1.1 Raman spectroscopy and XPS measurement 90
4.1.2 Result in APCVD 93
4.1.3 Role of oxygen in Rapid thermal Low-pressure chemical vapor deposition 97
4.1.4 Time evolution of graphene on all three sample 104
4.1.5 The JMAK fitting 108
4.1.6 Quantify the property of graphene grain 112
4.2 Artificial defect generates by Local anodic oxidation 117
4.2.1 AFM characterization 118
4.2.2 Micro-Raman spectroscopy 119
4.2.3 LAO speed test 121
Chapter 5 Conclusion 123
Reference 125
Appendix 133
C Code 133

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Appendix

指導教授

溫偉源(Wei Yen Woon)

審核日期

2016-7-21

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