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研究生： 陳鍾錡
Chung-Chi Chen
論文名稱： 硼摻雜石墨烯與金屬電極接面之光熱電效應
The Photo-thermoelectric Effect in the Contacts between Boron-doped Graphene and Metal Electrodes
指導教授： 周賢鎧
Shyankay Jou
口試委員: 黃柏仁
Bohr-Ran Huang
胡毅
Hu Yi
學位類別： 碩士
Master
系所名稱： 工程學院 - 材料科學與工程系
Department of Materials Science and Engineering
論文出版年： 2019
畢業學年度： 108
語文別： 中文
論文頁數： 161
中文關鍵詞： 石墨烯 、硼摻雜石墨烯 、場效電晶體 、電場效應量測 、聚焦雷射激發 、光熱電效應量測
外文關鍵詞： graphene, boron-doped graphene, field-effect transistor, electric field-effect measurement, focus laser beam excitation, photo-thermoelectric effect measurement
相關次數： 點閱：301  下載：1 
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    • 本研究主要分為三部份，首先以Cu(B)薄膜作為硼摻雜來源，透過快速升溫化學氣相沉積系統(Rapid thermal chemical vapor deposition system, RTCVD)來成長出硼摻雜石墨烯(Boron-doped graphene, BG)，並進一步優化製程參數與步驟來成長出品質優異的純石墨烯(Pristine graphene, PG)以比較兩者之性質差異。由SEM及拉曼光譜來比較製程調配結果，再由拉曼光譜、UV-vis光譜、XPS能譜以及SIMS質譜來分析兩者之材料特性。由拉曼光譜可以觀察到BG由於有硼摻雜進入石墨烯晶格中，造成晶格扭曲而使其缺陷較多。導致其D-band與D’-band的強度皆較高，2D-band則變寬且強度下降。搭配UV-vis光譜之穿透度結果推論PG為高品質單層石墨烯，而BG為多層硼摻雜石墨烯。XPS能譜與SIMS質譜之分析結果再次驗證了上述分析結果，並進一步提供了硼成功摻雜進入BG的證據。

    第二部份著重元件量測，將PG與BG應用於背閘極式石墨烯電晶體。在電性分析中確定了石墨烯與金屬電極為歐姆接觸，但量測出的電阻率明顯高於預期、載子遷移率亦明顯低於預期。同時亦無法透過閘極電壓掃描來獲得石墨烯之狄拉克點，結果呈現石墨烯有嚴重的p型摻雜。接續以聚焦雷射激發石墨烯通道中心、金屬電極與石墨烯接面處來量測光熱電效應。雷射的激發與否說明了元件對光有響應；而當由聚焦雷射以固定間距對石墨烯通道掃描時發現，在激發石墨稀通道與金屬電極接面處時，鈦銀電極接面處的通道電流會高於鋁電極接面處之通道電流，兩者之通道電流皆明顯高於僅激發石墨烯中心時的通道電流，證實在金屬電極與石墨烯接面處有光熱電效應產生。

    最後則對電晶體的製備作探討，希望由確保石墨烯品質與連續性、減少p型摻雜以及通道面積重新設計來增加電晶體的良率，以期量測出狄拉克點並應用於載子密度與賽貝克係數的計算。

    This study can be divided into three parts. Firstly, the Cu(B) thin film is used as a source of boron doping. Boron-doped graphene (BG) is grown by the rapid thermal chemical vapor deposition system (RTCVD), and the process parameters are further optimized to gain better quality graphene. Pristine graphene (PG) is used to compare the properties difference between the two. The results of the process renovation were checked by SEM and Raman spectroscopy, and the material properties of the graphene films were analyzed by Raman spectroscopy, UV-vis spectrometer, XPS, and SIMS. The results from Raman spectroscopy show that boron is doped into the graphene lattice due to boron doping, resulting in lattice distortion and more defects. Consequently, the intensity of both D-band and D'-band is higher, 2D-band is widened and the intensity is lowered. With the transmittance results of UV-vis spectra, PG is proven to be high-quality single-layer graphene, and BG is a multilayer boron-doped graphene. The analysis results of the XPS and SIMS verified the analysis results above and the evidence that boron was successfully doped into BG has been confirmed.

    The second part focuses on the device measurement, applying PG and BG to the back-gated graphene transistor. In the electrical analysis, the graphene and the metal electrodes were determined to be in ohmic contact, but the measured resistivity was significantly higher than expected, and the carrier mobility was also significantly lower than expected. At the same time, the Dirac point of graphene cannot be obtained by gate voltage sweeping, and the result shows that graphene has a heavy p-type doping condition. The photo-thermoelectric effect is measured by focusing the laser beam to excite the center of the graphene channel as well as the contacts between graphene and metal electrodes. The excitation of the laser beam indicates that the device is responsive to light; and when scanning the graphene channel at a fixed pitch with a focused laser beam, it is found that the channel current at the contact of the titanium/silver electrode and graphene is the highest. The channel current at the contact of the aluminum electrode and graphene is also higher than that of the channel current when only the graphene is excited. It is confirmed that a photo-thermoelectric effect occurs at the contacts between the metal electrodes and the graphene.

    Finally, the process of transistor fabrication is reviewed. It is hoped that the quality and continuity of the graphene, the reduction of the p-type doping and the channel area redesign will increase the yield of the transistor, in order to measure the Dirac point voltage and apply it to the calculations of carrier concentration and the Seebeck coefficient.

    摘要 I Abstract III 誌謝 V 目錄 VII 圖目錄 X 表目錄 XVI 第1章、 前言 1 1.1 石墨烯的起源與簡介 1 1.2 研究動機 3 第2章、 文獻回顧 4 2.1 石墨烯的結構及性質 4 2.2 石墨烯的製備方法 7 2.2.1 機械剝離法(Mechanical exfoliation) 7 2.2.2 磊晶成長法(Epitaxial growth) 8 2.2.3 氧化石墨烯還原法(Reduction of graphene oxide) 8 2.2.4 化學氣相沉積法(Chemical vapor deposition, CVD) 9 2.2.4.1 銅金屬觸媒成長石墨烯之機構 9 2.2.4.2 影響石墨烯成長及品質之參數 12 2.2.4.3 快速升溫化學氣相沉積法(Rapid Thermal Chemical Vapor Deposition, RTCVD) 16 2.3 石墨烯轉移 17 2.4 摻雜石墨烯 19 2.5 石墨烯電晶體製備及其電性量測 25 2.5.1 石墨烯電晶體之開關電流比值關係 28 2.5.2 氧化層電容與介電常數之關係 28 2.6 石墨烯之光熱電效應 29 第3章、 實驗儀器與實驗方法 40 3.1 實驗材料與藥品規格 40 3.2 實驗儀器及分析設備 42 3.3 實驗原理 43 3.3.1 化學氣相沉積系統(Chemical vapor deposition system, CVD) 43 3.3.2 微波電漿系統(Microwave plasma system, MWP) 43 3.3.3 磁控濺鍍系統(Magnetron sputtering system) 44 3.3.4 拉曼光譜顯微技術(Raman spectromicroscopy) 44 3.3.5 紫外光可見光光譜儀(Ultraviolet-visible spectrometer, UV-vis) 45 3.3.6 化學分析電子能譜儀(Electron spectroscopy for chemical analysis system, ESCA) 46 3.3.7 電晶體性質量測系統 47 3.3.8 二次離子質譜儀(Secondary ion mass spectrometer, SIMS) 49 3.4 實驗步驟 50 3.4.1 實驗步驟與分析 50 3.4.2 基板清洗 50 3.4.3 石墨烯成長 51 3.4.4 石墨烯轉移至特定基板 54 3.5 背閘極式石墨烯電晶體製備 56 3.5.1 電晶體元件及光罩設計 56 3.5.2 元件背閘極製備 57 3.5.3 圖案化微影製程 57 3.5.4 氧氣微波電漿蝕刻製程 61 3.5.5 金屬化薄膜濺鍍製程 61 3.5.6 舉離製程(Lift-off process) 62 3.5.7 元件退火製程與黃銅背板黏接 63 第4章、 研究結果與討論 64 4.1 純石墨烯與硼摻雜石墨烯之成長條件及性質探討 64 4.1.1 預處理對銅箔表面形貌的影響 64 4.1.2 拉曼光譜分析結果討論 67 4.1.3 UV-vis光譜穿透度結果討論 72 4.1.4 XPS能譜分析結果討論 73 4.1.5 SIMS質譜分析結果討論 82 4.2 石墨烯基背閘極式電晶體元件量測 92 4.2.1 電性量測分析與結果討論 92 4.2.2 光熱電效應之量測分析與結果討論 97 4.3 元件量測不如預期之原因探討 101 4.3.1 微影製程定位對準之問題 101 4.3.2 電晶體中石墨烯通道的品質 103 4.3.3 石墨烯通道之p型摻雜影響 106 4.3.4 定義石墨烯通道時電漿蝕刻的不足 109 4.3.5 汲極源極與背閘極導通之疑慮 112 4.3.6 石墨烯通道面積設計的影響 114 第5章、 結論 115 參考文獻 117 附錄 125

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