自從發現石墨烯這種新穎且極具發展潛力的二維材料後，其相關的製備方法與應用端也逐漸地被開發出來，而因為其具有優異的電子特性、可撓性與高光穿透度等優點，故在透明導電薄膜與光電元件的開發與應用上十分值得期待。而在目前眾多石墨烯的製備方法中，以化學氣相沉積法於金屬觸媒材料上成長石墨烯薄膜，並轉移至其他目標基板上之方式，較能達到大面積、高導電性與高光穿透度等應用要求。因此，本研究試圖將化學氣相沉積法於銅箔基板與濺鍍銅薄膜於二氧化矽/矽基板所成長的石墨烯，以陽極接合轉印技術，將其轉移至Pyrex7740之玻璃目標基板上，在整個陽極接合轉印製程中不用像傳統轉移技術，必須使用高分子聚合物(PMMA或PDMS)當作石墨烯的保護層與犧牲層，而在石墨烯轉移完成後該高分子聚合物則必須去除的問題，故此製程不僅沒有高分子殘留問題，在轉移過後也僅需使用到少量之銅蝕刻液，即可蝕刻掉於玻璃目標基板表面上所殘留之銅原子。
　　本研究重點主要分為三大項目: (1) 以化學氣相沉積系統成長石墨烯於銅箔與二氧化矽/矽基板表面之銅薄膜上，並以調控甲烷碳源與氬氫(Ar/H2)混合氣(9:1)之輔助氣體間的比例，來控制石墨烯層數與品質之成長參數。經由拉曼光譜分析證實已可成長出I2D/IG比值為2.04 ~ 2.98，半高寬為38.47 cm-1 ~ 46.42 cm-1之單層石墨烯(Single-layer graphene, SLG)，以及I2D/IG比值為0.51 ~ 0.66，FWHM為64.16 cm-1 ~ 73.57 cm-1之寡層石墨烯(Few-layer graphene, FLG)；(2) 由於在透明導電薄膜等應用上，FLG較能達到其元件應用之需求，故在實驗上則採用FLG來當作轉移之試片。並以開發的陽極接合轉印技術，將成長好的FLG從銅觸媒材料上轉移至面積尺寸為1 × 1 cm2之Pyrex玻璃目標基板，並透過調控其製程溫度以及工作電壓來達到轉移石墨烯之目的。經實驗結果顯示，於銅箔上成長的FLG，在製程溫度為150 ℃，工作電壓為0.9 kV為本實驗之最佳條件，其可在不需使用銅蝕刻液的情況下成功地轉移石墨烯，並在10 × 10 m2之範圍內，經拉曼映射及影像二值化分析軟體進行分析後，可得到其轉移率約為64.7%。而在以濺鍍而成之銅薄膜上，所成長出來的FLG，則是在工作電壓為0.6 kV，溫度為300 ℃之製程溫度下為最佳條件，在此條件可成功地轉移銅薄膜/石墨烯於Pyrex玻璃目標基板上，並且搭配0.1 M少量之銅蝕刻液去除表層的銅薄膜後，在10 × 10 um2之範圍內，以拉曼映射與影像二值化分析軟體進行分析，可得到其轉移率約為89.6%；(3) 本研究除了開發陽極接合轉印技術外，為了提升本技術之應用性，除了實驗之石墨烯轉移外，還利用濺鍍於二氧化矽/矽之銅薄膜與半導體製程進行整合，利用黃光微影、物理氣相沉積濺鍍與掀離等製程，進行尺寸大小為80 × 80 um2之方形陣列結構的圖案化定義，並接續進行前述石墨烯成長與轉移之最佳參數，將可實現快速且低成本之批量生產與產業應用。

Since the discovery of two-dimensional material graphene which has potential development, the production method and correlative application of grapheme are gradually being developed. Furthermore, because of extraordinary electrical feature, flexibility and high transmittance etc., we are looking forward developing and applying graphene to the transparent conductive film and the optoelectronics device. At the current stage, compared to other production methods, chemical vapor deposition is a better way to grow the graphene film on the metal catalyst material and transfer to the other target substrate for more application requirements, such like large area, high conductivity and high transmittance.
This research targeted at using anodic bonding transfer technology to transfer the graphene, grown on copper foil and sputtered copper with the way of chemical vapor deposition system, onto a 7740 Pyrex glass. During the whole process, it is not necessary to use polymer as the coverage and sacrifice layer, so this way solves the problem that traditional method would faces. Hence, there is not only no polymer residue at the end of the process but also cut down the amount of copper etching solution that etches the residue of copper atoms on the Pyrex glass.
This study is divided into three main items: (1) Growing graphene on copper foil and sputtered copper by chemical vapor deposition system, and to regulate the methane carbon and hydrogen mixture of argon gas (9: 1) the ratio between the auxiliary gas to control the growth parameters of graphene. In Raman spectroscopy, the I2D / IG ratio and FWHM are 2.04 ~ 2.98 and 38.47 cm-1 ~ 46.42 cm-1 for the single-layer graphene(SLG), the I2D / IG ratio and FWHM are 0.51 ~ 0.66 and 64.16 cm-1 ~ 73.57 cm-1 for few-layer graphene(FLG). (2) Due to the transparent conductive film and other applications, FLG is better able to achieve their application demand, so it is used in this experiment as the test piece for transfer. Moreover, this study through controls process temperature and operating voltage to transfer the FLG which grows on copper foil onto the 1 × 1 cm2 Pyrex glass by anodic bonding transfer technology to achieve the transfer of graphene purposes. The experimental results show that FLG growth on copper foil can be successfully transferred without using the copper etchant. Moreover, in the range of 10 × 10 um2, using Raman mapping and binary analysis software to analysis can obtain that the better rate of graphene transferred is about 64.7% at the process temperature of 150 ℃ and operating voltage of 0.9 kV. Furthermore, the FLG growth on sputtered copper can be successfully transferred by using the 0.1 M copper etchant. Moreover, in the range of 10 × 10 um2, using Raman mapping and binary analysis software to analysis can obtain that the better rate of graphene transferred is about 89.6% at the process temperature of 300 ℃ and operating voltage of 0.6 kV; (3) In addition to developing anodic bonding transfer technology, in order to enhance the applicability of this technology, in this study integrates sputtered copper semiconductor process by using photolithography, physical vapor deposition and lift-off to define the size of 80 × 80 um2 for the patterned square array structure. Moreover, using from the previous better parameters of graphene growth and transfer will realize quickly and low-cost for production and industrial applications.

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