石墨烯為單一碳原子層所組成之二維平面蜂巢狀石墨，具備有天然的二維電子氣系統。石墨烯不僅具有強韌的機械性質，其特殊的線性能帶結構，使得於其中傳導之載子表現為零質量之迪拉克費米子，同時具備有極優異的載子傳導特性。石墨烯的發現不僅提供了一個絕佳的二維傳輸系統，蘊含著豐富有趣的物理現象之外，在電子光電產業的應用上，更是眾所矚目的材料。目前製備石墨烯的主要方法是利用化學氣相沉積的方式大面積地成長於銅箔表面上。本論文將逐步探討石墨烯的電子傳輸特性、拉曼光譜分析以及化學氣相沉積石墨烯之材料分析。此外，本論文利用自然氧化之鋁電極，製作出自我對準閘極石墨烯場效電晶體，與傳統上閘極電晶體相比，其元件特性顯著提升，且其簡易製作、條件限制低之特性，可將石墨烯電晶體擴展至軟性電子之應用上。最後，經由精確的調控成長參數後，本論文可成長出雙層單晶石墨烯結構，具有不同的旋轉角度堆疊可能性。再利用拉曼光譜以及電子顯微鏡之分析，便可探討不同旋轉堆疊石墨烯的拉曼光譜特性。本論文之研究希望石墨烯在電子或光學元件的製備與應用上具有一定的貢獻。

Graphene, a single atomic layer of graphite comprising a planar two-dimensional hexagonal lattice of carbon atoms, is the building block for graphitic materials of all other dimensionalities. Based on the Mermin-Wagner Theorem, two-dimensional crystals were thermodynamically unstable and could not exist in ambient environment.The atomic monolayer materials have so far been known only as an integral part of larger three-dimensional structures. In 2004, A. K. Geim and K. S. Novoselov et al. provided a possible method to isolate two-dimensional single atomic carbon layer on SiO2 by using the mechanical cleavage of highly oriented pyrolytic graphite (HOPG).Since then, graphene has become an important research topic in the field of materials science and condensed-matter physics due to its unique properties. For instances, graphene has a host of characteristics that show great promise for the development of post silicon electronics,including a large room-temperature carrier mobility (20,000 cm2/V•s) and long-range ballistic transport.In addition to electrical properties, graphene is also an highly transparent material with an absorption of ∼ 2.3 % in visible light range Its thermal conductivity is measured to be ∼ 5,000 W mK-1 for a monolayer graphene at room temperature. The intrinsic mechanical properties of free-standing monolayer graphene are examined with the breaking strength of 42 N m-1 and the Young’s modulus of 1.0 TPa, indicating that it is one of the strongest materials ever measured.

This thesis focuses on the electrical and optical properties of graphene, including the synthesis, material characterizations and device applications. The first part presents the fabrication of graphene electronic devices, starting from the graphene synthesis by chemical vapor deposition (CVD), and the improvement of the device geometry in top-gate field-effect transistor (FET), addressing its emerging applications in flexible electronics. The second part presents the characterization of single-crystal graphene, which exhibits a high crystalline quality examined by transport analysis. We also study the fundamental issue of interlayer coupling between two rotational single-crystal bilayer graphene, which provides insights into the unique energy spectra of the two-dimensional carbon electron systems and may pave the way toward the opto-electronic applications.

Chapter 1 starts with the fundamentals of graphene, including the crystal structures as well as its energy band structure. The transport properties such as electric field-effect, minimum conductivity and scattering mechanism within graphene have been explained briefly. Chapter 2 presents an introduction of the Raman scattering, which is an important tool to examine the quality of graphene. We introduce the basic knowledge of Raman scattering and the phonon dispersion relation of graphene. Some extended studies such as electron-phonon coupling and doping effect have also been discussed. In Chapter 3, the characterization of polycrystalline graphene, such as Raman, transmission electron microscopy (TEM) and transport analysis have been presented. In order to improve the quality of graphene, we use the diluted concentration of hydrocarbon as precursor. This helps the self-limiting growth during the early stage of the growth on Cu. Single-crystal graphene can reduce the grain boundary scattering in micrometerscale electronics devices, which can enhance the device performance remarkably. In Chapter 4, a facile fabrication process for high-performance CVD graphene FETs with self-aligned drain/source contacts have been presented. In our process, an Al gate was directly defined on graphene by e-beam lithography, followed by air exposure or electrical annealing, forming a native oxide layer around the Al wire. We also characterize other device properties, such as charge neutrally point shifting, current saturation, and the complementary logic gate demonstration. Chapter 5 describes the fabrication of high-mobility low-voltage graphene FET array on a flexible plastic substrate using high-capacitance natural aluminum oxide as a gate dielectric in a self-aligned device configuration. The native aluminum oxide is resistant to mechanical bending and exhibits self-healing upon electrical breakdown. These results indicate that self-aligned graphene FETs can provide remarkably improved device performance and stability for a range of applications in flexible electronics. In Chapter 6, we present the study of the single-crystal bilayer graphene grown by ambient pressure CVD on polycrystalline Cu. Controlling the nucleation in early stage of growth allows the constituent layers to form single hexagonal crystals. New Raman active modes are shown to result from the twist, with the twist angle determined by the TEM analysis. The successful growth of single-crystal bilayer graphene provides an attractive jumping-off point for systematic studies of interlayer coupling in misoriented few-layer graphene systems with well-defined geometry.

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