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研究生： 張宏昱
Hung-Yu Chang
論文名稱： 以前驅物溶液塗佈法進行具二維結構之鈣鈦礦薄膜並應用於紅光發光二極體
Preparation of Two-Dimensional Perovskite Thin Films via Precursor Solution Coating Method for Application in Red-Emitting Light-Emitting Diodes
指導教授： 陳良益
Liang-Yih Chen
口試委員: 李坤穆
蘇子森
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： 2023
畢業學年度： 111
語文別： 中文
論文頁數： 164
中文關鍵詞： 銫鉛溴碘鈣鈦礦 、紅光發光二極體 、二維結構 、鹼金族碘鹽
外文關鍵詞： cesium lead bromide iodide perovskite, red-emitting light-emitting diodes, two-dimensional structure, alkali metal iodide
相關次數： 點閱：248  下載：0 
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    • 近年來，全無機鈣鈦礦薄膜在光電領域有巨大的突破，特別是三維與二維結構材料更是顯著提升鈣鈦礦薄膜的螢光表現進而提升發光二極體之性能。在本研究主要探討如何以銫鉛溴碘鈣鈦礦奈米結構薄膜製備發光波段位於650奈米的紅光發光二極體。首先，為了有效提升鈣鈦礦發光層的激子再結合，在此藉由添加苯乙基碘化銨與苯乙基溴化銨來形成具有二維結構的銫鉛碘與銫鉛溴碘鈣鈦礦薄膜做為發光層。由分析結果可知：於添加80%的苯乙基溴化銨(相對於碘化鉛)所製作的銫鉛溴碘鈣鈦礦發光二極體，其外部量子效率約為 1.09%。但是此發光二極體的發光波段位於668奈米。為了進一步調整二極體的發光波段，在前驅物溶液的成份配製方面，以溴化銫取代部份的碘化銫。當碘化銫：溴化銫=0.4：0.6時，所製備薄膜的發光波段調整至648奈米。此外，在本研究中，亦探討添加鹼金屬碘鹽對於銫鉛溴碘鈣鈦礦薄膜的螢光性質有何影響。由分析結果可知：當添加2毫克的碘化鋰於前驅物溶液時，銫鉛溴碘鈣鈦礦薄膜的螢光量子產率可達到20.33%，且將此鈣鈦礦奈米薄膜做為發光層時，所製備的發光二極體，其啟動電壓 為3.1 V，發光波段為648奈米，最大輝度值可達 978.4 cd/m2，電流效率為 1.77 cd/A以及外部量子效率可達3.57%。

    In recent years, there have been significant breakthroughs in the field of optoelectronics with all-inorganic perovskite thin films, especially with the use of three-dimensional and two-dimensional structured materials, which greatly enhance the fluorescence performance of perovskite thin films and improve the performance of light-emitting diodes (LEDs). In this study, the focus is on how to prepare red-light-emitting diodes with a emission wavelength of 650 nm using cesium lead bromide iodide (CsPb(Br/I)3)perovskite thin films. Firstly, in order to effectively enhance the exciton recombination of the perovskite emission layer, cesium lead iodide (CsPbI3) and CsPb(Br/I)3 thin films with a two-dimensional structure were formed by adding phenylammonium iodide (PEAI) and phenylammonium bromide (PEABr) to serve as the emission layer. Analysis results showed that the external quantum efficiency (EQE) of the CsPb(Br/I)3 perovskite LED (PeLED), prepared with the addition of 80% PEABr (relative to lead iodide), was approximately 1.09%. However, the emission wavelength of this PeLED was at 668 nm. In order to further adjust the emission wavelength of the PeLED, the composition of the precursor solution was modified by partially replacing cesium iodide (CsI) with cesium bromide (CsBr). When the ratio of CsI to CsBr was 0.4 : 0.6, the emission wavelength of the prepared thin film was adjusted to 648 nm. Furthermore, this study also investigated the effect of alkali metal iodides on the fluorescence properties of CsPb(Br/I)3 perovskite thin films. Analysis results showed that when 2 mg of lithium iodide (LiI) was added to the precursor solution, the photoluminescence quantum yield (PLQY) of the CsPb(Br/I)3 perovskite thin film achieved 20.33%. When this perovskite thin film was used as the emission layer, the prepared LED had a turn-on voltage of 3.1 V, an emission wavelength of 648 nm, a maximum luminance of 978.4 cd/m2, a current efficiency of 1.77 cd/A, and an EQE of 3.57%.

    中文摘要 5 Abstract 6 致謝 8 圖目錄 13 表目錄 23 第一章、 緒論 25 1-1 前言 25 1-2 研究動機與目的 26 第二章、 理論基礎 27 2-1 半導體與奈米結構 27 2-1-1 半導體材料 27 2-1-2 量子侷限效應與量子阱結構 29 2-2 半導體與奈米結構 31 2-2-1 鈣鈦礦結構 31 2-2-2 二維鈣鈦礦(2D perovskite) 34 2-2-3 鈣鈦礦材料的發展 36 2-3 鈣鈦礦發光二極體 39 2-3-1 發光二極體與各結構層之功能 39 2-3-2 發光二極體的工作原理 42 2-3-3 載子傳輸材料的選擇 43 2-3-4 發光二極體之效能指標 45 2-4 鈣鈦礦發光二極體近期研究與製程優化 55 2-4-1 降低鈣鈦礦晶體尺寸 55 2-4-2 金屬鹵化物修飾 58 2-4-3 近期鈣鈦礦發光二極體整理 62 第三章、 實驗設計 63 3-1 實驗流程圖 63 3-2 實驗藥品 64 3-3 實驗分析儀器與原理 68 3-3-1 紫外光-可見光光譜儀(UV/visible spectrophotometer) 68 3-3-2 絕對量子效率量測系統 69 3-3-3 X光繞射分析儀(X-ray Diffraction，XRD) 70 3-3-4 時間解析光致發光測量系統(Time-resolved photoluminescence，TRPL) 72 3-3-5 X光光電子能譜儀 (X-Ray Photoemission Spectroscopy，XPS) 73 3-3-6 紫外光電子能譜儀（Ultraviolet Photoelectron Spectroscopy，UPS） 74 3-3-7 低能量反轉光電子能譜儀 (Low Energy Inverse Photoelectron Spectroscopy，LEIPS) 76 3-3-8 高解析度場發射型掃描式電子顯微鏡 (High Resolution Field-emission Scanning Electron Microscope，FE-SEM) 77 3-3-9 電致發光量測系統(Electroluminescence，EL) 78 3-4 實驗步驟 80 3-4-1 氧化鎳前驅溶液製備 80 3-4-2 鈣鈦礦紅光二極體前驅溶液製備 80 3-4-3 發光二極體的製備 82 3-4-4 電子主導元件的製備 84 3-4-5 電洞主導元件的製備 86 第四章、 結果與討論 90 4-1-1 探討2D/3D混合CsPbBrxI3-x紅光二極體之光電效能 90 4-2 2D/3D混合CsPbBrxI3-x紅光二極體之製程優化探討 108 4-2-1 添加不同比例CsBr對CsPbBrxI3-x紅光二極體之效能探討 108 4-2-2 添加不同濃度KI對CsPbBrxI3-x紅光二極體之效能探討 123 4-2-3 添加不同濃度LiI對CsPbBrxI3-x紅光二極體之效能探討 137 第五章、 結論 153 第六章、 參考文獻 155 附錄 164

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