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研究生: 徐偉華
Hsu, Wei-Hua
論文名稱: 雷射誘導石墨烯與MAPbI3鈣鈦礦複合材料之紙基紫外光感測器
Laser-Induced Graphene/MAPbI3 Perovskite Composites for Paper-Based UV Photodetectors
指導教授: 涂維珍
Tu, Wei-Chen
學位類別: 碩士
Master
系所名稱: 電機資訊學院 - 微電子工程研究所
Institute of Microelectronics
論文出版年: 2023
畢業學年度: 111
語文別: 中文
論文頁數: 87
中文關鍵詞: 雷射誘導石墨烯石墨烯鈣鈦礦紙基紫外光感測器
外文關鍵詞: laser-induced graphene, perovskite, paper-based, photodetector
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  • 近年來柔性電子元件發展迅速,同時在永續環保、環境友善等議題被 廣泛討論之際,能夠透過自然環境中源源不絕的天然碳源製備的雷射誘 導石墨烯成為了一個潛在選項,為可持續再生和低成本的電子元件創造了發展道路。
    本論文中提出了在大氣環境條件下透過雷射直寫方式在纖維素濾紙上製備雷射誘導石墨烯之技術,雷射誘導石墨烯技術有精準控制能量、靈 活彈性的圖案化、多種基板皆可應用等優點。實驗選擇濾紙作為感測器的基板,製備的元件即具有可撓性之特色,後續再透過簡易的溶液沉積製程, 將具高光吸收特性的 MAPbI3 鈣鈦礦材料與石墨烯結合,提升元件整體的 光電特性。除此之外,實驗設計純石墨烯與石墨烯/MAPbI3 鈣鈦礦為光吸收層,將分析兩種不同結構光電感測器的機制與特性。
    根據實驗結果證實透過雷射參數的最佳化所製備雷射誘導石墨烯具 有良好的導電性,並且在不添加鈣鈦礦材料的情況下所製備的元件展現 出對紫外光快速響應的能力。單純石墨烯光感測器在施加 5 V 偏壓、光功率密度 187.4 mW/cm2 下,元件可得到最高 16.3 mA/W 的光響應度。添 加 MAPbI3 鈣鈦礦材料後的複合材料元件,因鈣鈦礦的高吸收特性與石墨 烯快速的載子傳輸能力,除了在光吸收度有明顯提升外,材料之間存在的 有效光生電荷轉移、光閘效應,使元件具有更優異的光電特性。在施加 5V 偏壓、光功率密度 161.4 mW/cm2 下,光感測器最高的光響應度為 144.7mA/W,探測率為 5.64×108 Jones,最後也驗證了紙基柔性元件在彎曲 1000 次後仍具有優異的光感測能力。
    本實驗成功製備了石墨烯與石墨烯/MAPbI3 鈣鈦礦兩種結構的紫外 光電感測器,兩者皆具有優異的光感測特性,並證實透過結合雷射誘導石 墨烯/ MAPbI3 鈣鈦礦材料能有效提升光電感測器的表現,在紙基可撓式 元件的應用上提供了未來發展綠能元件的可能性。

    In this paper, a laser direct writing technique is proposed for the preparation of laser-induced graphene on cellulose filter paper under atmospheric conditions. The laser direct writing technique offers advantages such as precise control of laser energy, flexible patterning, and compatibility with various substrates. Due to the choice of filter paper as the substrate, the prepared photodetectors exhibit a great flexibility. Subsequently, a simple solution deposition process is used to combine the highly light-absorbing MAPbI3 perovskite material, enhancing the overall optoelectronic properties of the graphene/MAPbI3 perovskite UV photodetectors.
    According to the experimental results, it was confirmed that the laser-induced graphene prepared through the optimization of laser parameters exhibited excellent conductivity. The device prepared without the addition of perovskite materials already demonstrated rapid response to ultraviolet light. For the graphene photodetector, the highest photoresponsivity was 16.3 mA/W can be obtained under a bias voltage of 5 V and power density of 187.4 mW/cm2. After adding MAPbI3 perovskite on the graphene film, due to the high absorption characteristics of perovskite, the fast carrier transport ability of graphene, the obvious improvement in light absorption, the effective photogenerated charge transfer and the photogating effect makes the graphene/MAPbI3 perovskite photodetectors have excellent optoelectronic properties. Under a bias voltage of 5 V and an optical power density of 161.4 mW/cm2, the highest photoresponsivity was 144.7 mA/W, with a detectivity of 5.64×108 Jones. Finally, it was also confirmed that the paper-based flexible device retained its light sensing capability even after undergoing 1000 bending cycles.

    中文摘要I 致謝X 目錄XI 表目錄XV 圖目錄XVI 第一章 緒論1 1-1 前言1 1-2 研究動機1 第二章 原理3 2-1 石墨烯簡介3 2-2 石墨烯合成方法5 2-2-1 機械剝離法(Mechanical exfoliation) 6 2-2-2 氧化石墨還原法(Reduction of graphite oxide) 7 2-2-3 化學氣相沉積法(Chemical vapor deposition, CVD) 8 2-2-4 碳化矽外延生長法(SiC epitaxial growth) 9 2-3 雷射誘導石墨烯(Laser-induced graphene, LIG) 10 2-3-1 雷射誘導石墨烯形成機制12 2-3-1-1 使用CO2和長脈衝雷射12 2-3-1-2 使用短脈衝雷射14 2-3-2 雷射誘導石墨烯特點及應用15 2-4 鈣鈦礦材料介紹16 2-4-1 CH3NH3PbI3鈣鈦礦17 2-5 光電感測器原理19 2-5-1 光電導效應20 2-5-2 光閘效應20 2-5-3 光伏效應21 2-5-4 光熱電效應22 2-5-5 光輻射熱效應23 第三章 實驗材料與儀器24 3-1 實驗藥品及材料24 3-2 實驗儀器25 3-2-1 微量滴管25 3-2-2 電磁加熱攪拌器26 3-2-3 雷射雕刻機台27 3-2-4 惰性氣體手套箱28 3-2-5 高解析熱場發射掃描式電子顯微鏡29 3-2-6 拉曼光譜儀30 3-2-7 化學分析電子光譜儀31 3-2-8 光致發光光譜儀32 3-2-9 紫外光可見光/近紅外光分光光譜儀33 3-2-10 X光繞射儀34 3-2-11 電性量測系統35 第四章 實驗步驟36 4-1 光感測器製程36 4-2 基板預處理37 4-3 雷射誘導石墨烯製備37 4-4 鈣鈦礦薄膜38 4-4-1 鈣鈦礦前體溶液製備38 4-4-2 鈣鈦礦薄膜製備40 4-5 導電銀膠製備電極40 第五章 結果與討論41 5-1 前言41 5-2 掃描式電子顯微鏡分析(含元素分析) 41 5-2-1 雷射誘導石墨烯轉化過程41 5-2-2 雷射誘導石墨烯與MAPbI3複合材料45 5-3 拉曼光譜分析47 5-4 XPS元素分析50 5-5 XRD晶相分析52 5-6 光致發光光譜分析53 5-7 UV-vis吸收光譜分析55 5-8 元件操作機制57 5-9 I-V電流電壓量測分析59 5-10 光響應度與光電流分析63 5-11 探測率分析67 5-12 元件開關燈響應分析71 5-13 外部量子效率分析75 5-14 元件可撓度分析77 第六章 結論及未來研究方向79 參考文獻80

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