本論文之研究主要在探討石墨烯及其衍生物的成長機制，包括單層雪花狀石墨烯，多孔多層石墨烯，奈米碳管成長於多孔多層石墨烯之複合物，以及多層站立之石墨烯奈米牆。首先，以銅箔為催化劑，利用化學氣相沉積法在銅箔上成長大面積的單層石墨烯，其大小超過0.5平方公厘。本研究藉由拉曼光譜以及電子顯微鏡等材料分析技術，證明石墨烯在越長越大的過程中，即使受到銅箔催化成長，其晶體方向並不會因為遇到底下的銅晶界而更改晶體方向(Orientation)，但可能會改變其成長方向(growth front)。並藉由量測石墨烯的電子遷移率驗證，有通過銅晶界及沒有通過的雪花分支，兩者電子遷移率沒有太大差異。主要原因推測是在成長過程中，接近銅熔點的高溫下，在晶粒表面銅原子並沒有與石墨烯的碳原子有很強的鍵結，因此不會主導石墨烯的晶體方向。本論文也同時探討了石墨烯與銅晶粒的原子排列結構關係。
除此之外，我們也發展出一種方法置備空心奈米碳棒以及多孔石墨烯的複合物。首先利用固體擴散法成長具有多孔性的石墨烯薄膜，再以此為基板，在未使用任何金屬催化劑情況下，利用化學氣相沉積法在其上成長空心奈米碳棒。置備多孔石墨烯基板主要分成兩個步驟：一，先在矽晶板上鍍上非晶質的碳膜，在其上鍍上鎳金屬薄膜做為催化劑；二，藉由高溫退火後，碳原子會由鎳晶界擴散至鎳薄膜表面形成石墨烯。由於高溫退火時，鎳晶粒成長，會形成空孔，這些空孔則做為多孔石墨烯的模板。分析所得的複合物，發現大部分空心奈米碳棒沿著石墨烯空孔的邊緣成長，推測石墨烯空孔的邊緣具有許多的碳懸鍵(dangling bond)，可以做為奈米碳棒成長的成核點。本論文也利用拉曼及電子顯微鏡對所合成出來的多空石墨烯以及複合物分析，並探討兩者的成長機制。
最後，本論文還闡述直接在單晶矽基板上成長石墨烯奈米牆的可能性。根據實驗結果，發現(100)單晶矽基板，在預處理過程中，{100}的表面會被離子化的氫氣蝕刻後產生許多{111}的奈米級平面。透過高解析穿透式電子顯微鏡，可以觀察到由AA-stacked多層石墨烯奈米牆的晶格條紋與矽{111}的晶格條紋相接，顯示石墨烯奈米牆可以直接成核於矽{111}平面上，並繼續成長。而非晶質的碳與碳化矽奈米顆粒則被發現沉積於其他的矽晶面上。這是由於石墨烯奈米牆與矽的晶格不匹配系數非常小，因此兩者可以異質磊晶成長。

The aim of this research is to investigate the growth mechanism of the synthesis of graphene related materials by various methods. The graphene related materials include monolayer graphene snowflake, porous graphenic carbon film, composite of carbon nanorod on porous graphenic carbon film, and graphene nanowalls.
First, chemical vapor deposition is employed to grow large single-domain graphene snowflakes (> 0.5 mm2) on Cu foil by crossing numerous Cu grain boundaries underneath. The orientation of the graphene snowflake branches is preserved when crossing the Cu grain boundaries, as evidenced by Raman spectra and transmission electron microscopy analysis. Diffraction patterns and scanning electron microscopy images reveal a relationship between the growth front and the orientation of graphene snowflakes. The graphene snowflake branch portions before and after crossing a Cu grain boundary show similar effective field-effect mobilities, confirming that the orientation did not change. Diffraction patterns of graphene and electron backscattering diffraction maps of Cu grains are used to study graphene lattice overlap below Cu grains. The orientation of Cu grains has little influence on the growth of top graphene snowflakes, probably due to the weak bonding interaction between Cu grains and graphene, constraining the growth of graphene snowflakes at temperatures close to the melting point.
Second, a method is developed for growing three-dimensional hierarchic structures of porous graphenic carbon film/ hollow carbon nanorods where porous graphenic carbon film is first synthesized followed by, growth of carbon nanorods. Porous graphenic carbon films were synthesized by solid-state diffusion on nickel thin film. By annealing an amorphous carbon layer deposited underneath a nickel thin film at elevated temperatures, the porous graphenic carbon film forms on top via carbon diffusion and precipitation from the grain boundaries of the nickel film. Hollow carbon nanorods can then be grown on the pore edges of the porous graphenic carbon film by chemical vapor deposition without catalysts. It is speculated that the dangling bonds of the carbon atoms on the pore edges of the graphene layers might be responsible for the nucleation of the hollow carbon nanorods. The microstructures and growth mechanisms of both porous graphenic carbon film and hollow carbon nanorods are characterized and discussed in detail.
Finally, carbon nanowalls were successfully grown on Si(001) wafer by direct-current plasma enhanced chemical vapor deposition. Carbon nanowalls, standing structure of graphene sheets, are vertical to substrate. Heteroepitaxial nucleation of {002} graphene sheets on {111} facets of plasma treated (100) silicon is confirmed by high-resolution transmission electron microscopy. Lattice mismatch by 12% is compensated by tilting the graphene {002} with respect to silicon {111} and matching the silicon lattice with fewer graphene layers. The interlayer spacing of graphene sheets near the silicon surface is 0.355 nm, which is larger than that of AB stacked graphite and confirmed as AA stacked graphitic phase. A strong Raman peak corresponding to silicon-hydrogen stretch vibration is detected by 633 nm excitation at the early stage of graphene nucleation, indicating the silicon substrate etched by hydrogen plasma. With these analyses, the growth mechanism is also proposed.

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