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研究生： 洪祐謙
YU-CHIEN HUNG
論文名稱： 鈣鈦礦發光二極體
Perovskite Light-Emitting Diode
指導教授： 陳良益
Liang-Yih Chen
口試委員: 陳貞夙
Jen-Sue Chen
吳季珍
Jih-Jen Wu
邱智瑋
Chih-Wei Chiu
學位類別： 碩士
Master
系所名稱： 工程學院 - 化學工程系
Department of Chemical Engineering
論文出版年： 2020
畢業學年度： 108
語文別： 中文
論文頁數： 140
中文關鍵詞： 溴化銫鉛 、鈣鈦礦 、發光二極體 、聚乙二醇
外文關鍵詞： cesium lead bromide, perovskite, light-emitting diode (LED), polyethylene glycol (PEO)
相關次數： 點閱：294  下載：0 
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    • 無機鹵化銫鉛鈣鈦礦因具有成本低、可調節發光波段、半高寬窄和螢光量子效率高等優點，近來多應用於顯示器研究。在本研究中，以兩種不同的方法製作溴化銫鉛鈣鈦礦薄膜，應用於發光二極體並分析其光電特性。第一種方法於鈣鈦礦前驅液添加不同比例的聚乙二醇(分子量：100,000 g/mol)，探討添加量對溴化銫鉛鈣鈦礦薄膜的成膜影響；第二種方法則是先合成溴化銫鉛粉體後，再將此粉體與不同比例的溴化銫混合配製成前驅溶液進行薄膜製備。以上兩種方式所塗佈的薄膜經分析可知：以添加聚乙二醇的鈣鈦礦前驅液能塗佈出覆蓋性較佳的溴化銫鉛鈣鈦礦薄膜，其載子平均生命週期為13.77 ns。之後，將此溴化銫鉛鈣鈦礦薄膜塗佈條件應用於發光二極體研究中，並以氧化銦錫基板、聚(3,4-亞乙二氧基噻吩)-聚(苯乙烯磺酸)、1,3,5-三(1-苯基-1H-苯并咪唑-2-基)苯、氟化鋰與鋁分別做為發光二極體結構中的陽極、電洞注入層/傳輸層、電子傳輸層、電子注入層與陰極。由發光二極體的特性研究可得知：使用15 Ω/sq氧化銦錫基板與電洞遷移率較低的聚(3,4-亞乙二氧基噻吩)-聚(苯乙烯磺酸) (Al 4083)可獲得較佳的元件性能表現。此外，在本研究中以溴化銫(0.15 M)與溴化鉛在莫耳比為3:2，並添加0.006克的聚乙二醇所配製的溴化銫鉛鈣鈦礦前驅液所塗佈的溴化銫鉛鈣鈦礦發光層，其組裝的發光二極體效能為：啟動電壓為 3.20 V，最大輝度為1330 cd/m2、最大電流效率為0.899 cd/A，外部量子效率為0.236%。

    Inorganic cesium lead halogen perovskite has the advantages of low cost, tunable light-emitting wavelength, narrow half-height width and high photoluminescence quantum yield. Recently, it has been used in display research in recent. In this study, two methods were used to coat cesium lead bromide (CsPbBr3) perovskite thin film for studying the optoelectronic properties of light-emitting diodes (LEDs). The first method is to add different amount of polyethylene glycol (PEO, molecular weight: 100,000 g/mol) to the perovskite precursor solution and to discuss the effect of the added PEO amount on the formation of CsPbBr3 thin film. The second method is to synthesize CsPbBr3 powders firstly. After that, the powders were mixed with different ratio of cesium bromide (CsBr) to prepare the precursor solution for CsPbBr3 thin film coating. According to analysis results of CsPbBr3 thin film coated by above two methods, we could observe that the first method could obtain good film coverage and its average carrier lifetime was 13.77 ns. In the next, this coating conditions of CsPbBr3 perovskite thin film were applied to the study light-emitting diodes and indium doped tin oxide (ITO) substrate, poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS), 1,3,5-Tris(1-phenyl-1H-benzimidazol-2-yl)benzene (TPBi) and lithium fluoride (LiF) and aluminum (Al) were used as anode, hole injection/transport layer, electron transport layer, electron injection layer and cathode. From the characteristics of the prepared CsPbBr3 perovskite LEDs, we could obtain that LED with 15 Ω/sq ITO substrate and PEDOT:PSS with low hole mobility (Al 4083) got better performance of device. In addition, the CsPbBr3 precursor solution prepared with cesium bromide (0.15 M) and lead bromide (PbBr2) in molar ratio of 3 : 2 and 0.006 g PEO was added for CsPbBr3 light-emitting layer coating. The performances of CsPbBr3 LDEs were as following: turn-on voltage was 3.20 V, the maximum brightness was 1330 cd/m2, the maximum current efficiency was 0.899 cd/A, and the external quantum efficiency was 0.236%.

    中文摘要 I Abstract III 致謝 V 目錄 VI 圖目錄 XI 表目錄 XIX 第一章、 緒論 1 1-1前言 1 1-2研究動機與目的 2 第二章、 理論基礎與文獻回顧 3 2-1半導體材料 3 2-1-1 n型半導體與p型半導體和pn-junction 6 2-1-2順向偏壓和逆向偏壓　9 2-2鈣鈦礦材料　12 2-2-1鈣鈦礦結構　13 2-2-2鈣鈦礦薄膜的製備　15 2-2-2-1 溶液法　15 2-2-2-2雙源氣相沉積(dual-source vapor deposition， DSVD)　17 2-2-2-3氣相輔助溶液法(vapor-asisted solution process)　18 2-2-3鈣鈦礦薄膜的優化　19 2-2-3-1溴化銫比例對鈣鈦礦薄膜影響　19 2-2-3-2添加高分子對鈣鈦礦薄膜影響　23 2-3發光二極體　27 2-3-1發光二極體機制與結構　27 2-3-2 發光二極體量測 30 2-3-2-1輝度與最大輝度(luminance and maximum luminance，Lmax) 30 2-3-2-2啟動電壓(turn on voltage，Von) 30 2-3-2-3電流效率(current efficiency，CE) 31 2-3-2-4外部量子效率(EQE，external quantum efficiency) 31 2-3-3 發光二極體設計 34 2-3-3-1電極的選擇 34 2-3-3-2電洞傳輸層/電洞注入層/電子阻擋層的優化 35 2-3-3-3電子傳輸層/電子注入層/電洞阻擋層優化 41 2-3-3-4 發光二極體各層能帶位置圖 44 2-4 近期間發光二極體元件整理 45 第三章、 實驗設計 47 3-1 實驗流程圖 47 3-2實驗藥品 48 3-3實驗儀器分析與原理 53 3-3-1紫外光/可見光光譜儀(UV/VIS spectrophotometer) 53 3-3-2螢光光譜儀 (fluorescence spectrophotometer) 54 3-3-3 X 光繞射分析儀 (x-ray diffraction，XRD) 55 3-3-4 時間解析螢光光譜儀(time-resolved photoluminescence，TRPL) 56 3-3-5 場發射掃描式電子顯微鏡(field-emission scanning electron microscope，FESEM) 57 3-3-6 接觸角量測儀(contact angle meter) 58 3-3-7 紫外光電子能譜(ultroviolet photoelectron spectrometer, UPS) 59 3-3-8 電致發光量測系統(electronluminance analysis system) 66 3-3-9 落球式粘度計(falling ball viscometer) 67 3-4實驗步驟 68 3-4-1 發光二極體製備 68 3-4-1-1定義工作面積和清洗基板 68 3-4-1-2塗佈電洞傳輸層/電洞注入層 69 3-4-1-3塗佈鈣鈦礦層 70 3-4-1-4蒸鍍電子傳輸層、電子注入層與電極 71 3-4-2 電洞主導元件 73 3-4-3電子主導元件 74 第四章、 結果與討論 75 4-1載子傳輸層材料特性分析 75 4-1-1 電洞傳輸層/注入層特性分析 75 4-1-2 電子傳輸層特性分析 85 4-1-3 電子注入層與陰極特性分析 87 4-2 CsPbBr3薄膜發光層製備與特性分析 88 4-2-1 鈣鈦礦前驅液添加不同比例PEO 88 4-2-2 CsPbBr3粉末回溶後添加不同比例CsBr 97 4-2-3 鈣鈦礦薄膜的選擇 106 4-3 以CsPbBr3作為發光層製備發光二極體及其光電特性分析 108 4-3-1 陽極ITO與PEDOT:PSS的選擇 108 4-3-2 鈣鈦礦濃度的調配與優化 115 4-3-3 電致發光元件注入平衡分析 124 4-3-4 發光元件穩定性分析 126 第五章、結論 128 第六章、參考文獻 129

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