傳統製備石墨烯之方法，其中之一為化學氣相沉積法，調配溫度、氣體流量、壓力與時間等參數，搭配金屬催化劑如銅箔、鎳箔等基材成長石墨烯，可有效成長、控制石墨烯的面積與層數。再透過轉移製程，將石墨烯薄膜轉移至目標基板上以進行後續元件製作。然而，轉移製程是一種破壞性步驟，使石墨烯在過程中容易受到汙染、破損，增加缺陷數量而降低其優異的特性。因此，去除轉移製程，避免轉移步驟造成損害，直接於目標基板上成長石墨烯的技術逐漸被重視與深入研究。
利用熱蒸鍍於氧化矽基板與石英基板上沉積銅膜，將銅膜當作金屬催化劑，使其在高溫退火環境中，銅膜表面產生變化形成孔洞並同時伴隨著甲烷裂解、碳原子沉積，於銅膜與氧化矽基板之間沉積石墨烯薄膜。藉由田口法規劃不同的退火時間與氣體流量，得到最佳的製程參數其成長出的石墨烯薄膜片電阻為274 Ω，遷移率為699 cm2/Vs；並利用影像分析的方式辨別銅膜退火後的表面狀態與銅膜成長石墨烯並進行蝕刻後的薄膜覆蓋率，分析結果當使用800 nm銅膜退火產生的孔洞大小約為27.9 μm2左右，孔洞密度為4.017x10-3/μm2時，得以成長出覆蓋率高達99.6 %的石墨烯薄膜。後續探討銅膜催化生長的成長機制為銅膜高溫下液化、蒸發產生孔洞，碳原子沉積於孔洞處並與周圍提供的銅蒸氣催化成長石墨烯，同時碳原子也由孔洞邊緣處擴散進入氧化矽與銅膜之間成長石墨烯。
本論文也針對直接成長免轉移石墨烯進行物理特性測試，如:熱穩定性、光學特性，其可見光穿透率為95.1 %。最終可應用於半導體元件微小化的製程中，利用圖形化定義銅膜面積，進而直接成長石墨烯於欲沉積的區域，有效節省微影步驟。

The traditional chemical-vapor-deposition method is to optimize process parameters on copper or nickel foils for graphene preparation. However, the transferring process to another substrate for device fabrication would degrade the performance due to the increase of defect amount. Therefore, direct synthesis of transfer-free graphene is the promising method for further device process.
In this thesis, copper films were deposited on SiO2 substrates (SiO2/Si) and quartz substrates by thermal evaporation as metal catalysts. When the Cu/SiO2/Si samples were annealed at the high temperature (1020 oC), Cu aggregated and some Cu voids were formed. At such a high temperature, methane pyrolysis acted as the carbon source to deposit graphene layers. Taguchi method with several process parameters, such as annealing temperature and gas flow rate, was used to optimize the graphene preparation. The image analyses with Cu voids after preliminary annealing process and after graphene growth, and images of graphene on SiO2/Si investigated the optimized process parameters and graphene growth mechanism. When void size was 27.9 μm2 and void density was 4.017x10-3 /μm2, the coverage ratio of graphene on SiO2/Si had the highest value of 99.6 %, which optimized the graphene properties with sheet resistance of 274 Ω and mobility of 699 cm2/Vs.
The thermal stability and optical property of graphene were also investigated. The sheet resistance of graphene kept almost the same in air at 200 oC for 60 min. The transmittance of the optimized graphene on quartz substrate was 95.1 %.

目錄
中文摘要 V
ABSTRACT VI
誌謝 VIII
目錄 IX
圖目錄 XI
表目錄 XIV
第一章 緒論 1
1-1 前言 1
1-2 動機與目的 1
1-3 論文架構說明 2
第二章 基礎理論與文獻回顧 3
2-1 奈米材料簡介 3
2-2 石墨烯 5
2-2-1 石墨烯介紹與應用 5
2-2-2 石墨烯物理特性 5
2-2-3 石墨烯製備方式 9
2-2-4 石墨烯檢測方式 13
2-3 化學氣相沉積製備石墨烯 18
2-3-1 化學氣相沉積製備石墨烯原理 18
2-3-2 催化金屬差異 22
2-3-3 氣氛濃度對製備影響 26
2-3-4 壓力對製備影響 29
2-3-5 溫度對製備影響 31
2-3-6 退火時間影響 32
2-3-7 銅膜厚度影響 33
2-4 直接成長與間接成長差異 35
2-4-1 直接成長 35
2-4-2 間接成長 36
2-5 田口方法介紹 38
第三章 實驗步驟與方法 40
3-1 實驗敘述與流程說明 40
3-2 實驗設備 41
3-3 石墨烯製備說明 42
3-4 銅蝕刻 45
3-5 材料分析 47
3-6 圖像分析 49
3-7 電性量測與物理特性 50
3-7-1 霍爾效應分析 50
3-7-2 石墨烯熱穩定性測試 52
第四章 結果與討論 53
4-1 銅膜催化成長石墨烯 53
4-1-1 石墨烯製備製程 54
4-1-2 蝕刻、清洗最佳化 64
4-1-3 不同基板成長 66
4-2 銅膜與石墨烯覆蓋率 67
4-2-1 銅膜不同厚度與退火時間變化 67
4-2-2 石墨烯覆蓋率 70
4-3 石墨烯特性與應用 77
4-3-1 石墨烯物理特性 77
4-3-2 圖形化應用 79
第五章 結論與未來展望 80
5-1 結果討論 80
5-2 未來展望 82
參考文獻 83

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