臺灣博碩士論文加值系統

氧化銦鎵鋅(IGZO)具有優良的電及光電特性，加上可見光之寬能隙值及高透明度是目前螢幕面板領域中最被看好的薄膜材料，本研究擬添加石墨烯來增強其性質，並期望藉由退火處理，能消弭薄膜內部殘留應力，改善其性質。
本論文利用化學氣相沈積法成長出高品質之石墨烯。首先探討石墨烯的電性、拉曼光譜分析以及內部結構缺陷的檢測，經過長時間的參數測試，成功長出高品質單層石墨烯。再使用轉印方法，將石墨烯轉印在聚醯亞胺(Polyimide, PI)基板上，接著使用磁控濺鍍的方式將鈦(Ti)與氧化銦鎵鋅(IGZO)沉積在石墨烯上，形成複合材料之堆疊。
本實驗利用四點探針與霍爾效應分析儀量測薄膜之電性，比較有無添加石墨烯之樣品，結果顯示有添加石墨烯樣品之片電阻值低於無添加石墨烯之樣品10倍以上，效果十分顯著。除此之外，載子遷移率也有明顯上升，量測結果顯示添加石墨烯會使薄膜之載子遷移率提升30~60%。接著利用奈米壓痕試驗機比較兩者之硬度，發現添加石墨烯能使整體硬度大幅提升，約上升了60%。
殘留應力(Residual Stress)與氧空缺比率(IRO2)是影響薄膜材料的機械、光學及電學性質的重要因子。本實驗比較常溫25oC與退火100oC、200oC、300oC各一小時之樣品氧空缺含量。發現當退火溫度增加時，IRO2隨之增加，同時內部的殘留應力也會隨著退火處理而被釋放。氧空缺的增加與殘留應力的減少將會大幅度地改善薄膜電性，使載子遷移率上升與電阻率下降。
本研究發現添加一層Ti有助於增加整體薄膜之電性與層與層之間的附著性。透過穿透式電子顯微鏡(TEM)與能量分散光譜儀(EDS)分析發現當退火時IGZO內部的氧離子會掙脫與In、Ga、Zn之間的束縛，與Ti形成鍵結。並透過退火處理後增加Ti的結晶性，使電性加強。退火處理同時也會影響薄膜之透光率。當退火溫度增加時，薄膜之結晶性變強，晶格排列更加整齊。當光照射時會減少光之散射，使透光率增加。

This thesis use CVD method to create high quality graphene. First, we investigate graphene quality by Raman Analysis, Four-Point Probe and microstructure analyses. After a long test, we have made a high quality single-layer graphene successfully, and use the wetting transfer method to transfer this graphene to polyimide substrate. At last, depositing Ti and IGZO on graphene/polyimide to prepare a composite film by Magnetron Sputter.
The results show that the sheet resistance of the samples with the graphene film is 10 times lower than that the samples without graphene. In addition, the carrier mobility also increased significantly, the results show that the use of graphene will elevate the carrier mobility by 30 to 60%. The application of nano-indentation system was found that the deposition of graphene can make a substantial rise in overall hardness about 60%.
In this experiment, the oxygen content of samples was measured at room temperature and 100 ℃, 200 ℃ and 300 ℃ for 1 hour. It was found the IRO2 increased and internal residual stress was lower by increasing the annealing temperature. The increase of oxygen vacancies and the decrease of residual stress can improve the electrical properties of the film greatly. The carrier mobility of the film increases and the resistivity of the film decreases significantly.
The results show that the addition of a layer of titanium increases the electrical properties of the thin film and the adhesion between the IGZO layer and the PI substrate and improve the electrical properties of IGZO. Besides, Annealing treatment affects the transmittance of the film. When the annealing temperature increases, the crystallinity of the film becomes stronger and the lattice arrangement is neater.

摘要 I
Extended Abstract III
致謝 VI
目錄 VII
表目錄 XII
圖目錄 XIV
第一章 緒論 1
1.1 前言 1
1.2 文獻回顧 3
1.3 研究目的 8
1.4 研究架構 9
第二章 基本理論 10
2.1 IGZO介紹 10
2.1.1 晶體結構 10
2.1.2 光學性質 11
2.1.3 導電性質 11
2.2 載子濃度、載子遷移率及電阻率之關係 13
2.3 石墨烯介紹 14
2.4 石墨烯基本性質 15
2.4.1 光學性質 15
2.4.2 電學性質 15
2.4.3 力學性質 16
2.5 石墨烯的製備方法 17
2.5.1 機械剝離法 17
2.5.2 氧化還原法 17
2.5.3 化學氣相沉積法 18
2.6 殘留應力理論 19
2.6.1 殘留應力簡介 19
2.6.2 殘留應力理論分析 20
2.6.3 晶粒大小理論分析 21
2.7 鈦對於IGZO的影響 22
2.8 儀器理論 22
2.8.1 磁控濺鍍(Magnetron Sputtering)原理 22
2.8.2 拉曼量測原理 23
2.8.3 掃描式電子顯微鏡原理 24
2.8.4 穿透式電子顯微鏡原理 26
2.8.5 光學原理 27
2.8.6 四點探針原理 28
2.8.7 霍爾量測原理 29
第三章 實驗流程 43
3.1 實驗目的 43
3.2 實驗步驟 44
3.2.1 銅箔前處理 44
3.2.2 成長石墨烯 45
3.2.3 石墨烯轉印(Graphene Transfer Method) 45
3.3 實驗設備 46
3.3.1 化學濕式操作台 46
3.3.2 共濺鍍機台 48
3.3.3 拉曼光譜儀 48
3.3.4 表面粗度儀 49
3.3.5 雙束型聚交離子束 50
3.3.6 穿透式電子顯微鏡 50
3.3.7 掃描式電子顯微鏡 51
3.3.8 四點探針 51
3.3.9 霍爾效應分析儀 51
3.3.10 原子力顯微鏡 52
3.3.11 奈米壓痕試驗機 52
3.3.12 X光繞射儀 53
3.3.13 分光光譜儀 53
3.3.14 橢圓偏光儀 54
3.3.15 化學分析電子光譜儀 54
第四章 結果與討論 69
4.1 石墨烯製程分析 69
4.2 石墨烯轉印方法(Graphene Transfer Method) 70
4.3 石墨烯檢測 72
4.3.1 拉曼光譜分析 72
4.3.2 TEM分析 73
4.3.3 XPS分析 74
4.3.4 AFM分析 75
4.3.5 四點探針分析 75
4.4 IGZO結構分析 76
4.4.1 FIB分析 76
4.4.2 XRD分析 77
4.4.3 晶粒大小分析 78
4.4.4 AFM分析 78
4.4.5 殘留應力分析 79
4.4.6 奈米壓痕分析 79
4.5 IGZO成分分析 80
4.5.1 XPS分析 80
4.5.2 EDS分析 81
4.6 IGZO光學分析 82
4.6.1 透光率分析 82
4.6.2 能隙值分析 82
4.6.3 反射率分析 83
4.6.4 折射率與消光係數分析 84
4.7 IGZO電性分析 84
4.7.1 電阻分析 84
4.7.2 霍爾量測分析 85
4.8 各性質之相關性 86
第五章 結論與未來展望 131
5.1 結論 131
5.2 未來展望 132
參考文獻 134

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