單源熱蒸鍍全無機鈣鈦礦薄膜與發光二極體之研究

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黃天賜(Tain-Shi Huang) 查詢紙本館藏

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機械工程學系

論文名稱

單源熱蒸鍍全無機鈣鈦礦薄膜與發光二極體之研究
(The Study of Single-source Vacuum Deposition of Inorganic Perovskite Thin Film and Light Emitting Diode)

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摘要(中)

全無機鹵化物鈣鈦礦材料，不僅具有良好的光電特性，還有良好的環境耐候性，因此大量的研究開始投入研究這個極具發展潛力的材料，將其用來提升太陽能電池與發光二極體等光電元件。目前大部分的製程以溶液旋塗法為主，但是薄膜的平整性及溶劑的汙染對元件影響極大，於是有人開始利用熱蒸鍍的方式製作。在本研究中我們亦選擇熱蒸鍍製程進行研究，不過有別於目前科學界常使用兩種原料的雙源共蒸鍍製程，我們則是利用單一蒸鍍源並且搭配CsPbBr3粉末，有效改善雙源共蒸鍍時必須很精準控制蒸鍍原料比例的問題。
本論文首先證明利用單源熱蒸鍍CsPbBr3粉末所得之薄膜品質優於單純將CsBr和PbBr2均勻混合的粉末；接著我們開始提升CsPbBr3薄膜的品質，改善薄膜中CsPbBr3的衍生相: CsPb2Br5與Cs4PbBr6，由於這兩者過量的存在可能會導致薄膜的電性變差，影響到發光二極體元件最終的效率，因此我們調整熱處理的溫度及時間，來消除薄膜中的衍生相，提升鈣鈦礦薄膜的品質，並且應用在發光二極體中。
除此之外，目前大部分的鈣鈦礦發光二極體之電子傳輸層與電洞傳輸層，仍使用有機材料，這些材料除了環境耐候性差以及價格昂貴之外，不論在製造還是丟棄時，對環境都有很大的污染性，為了改善這個問題，本研究採用低環境汙染、價格便宜且耐候性佳之氧化鋅與氧化鉬等金屬氧化物來取代有機電子傳輸層與電洞傳輸層，經過UPS的量測確定能階後，將其作為發光二極體的電子、電洞傳輸層。
本論文利用單源熱蒸鍍法製作高品質之鈣鈦礦(CsPbBr3)主動層薄膜，並藉由熱蒸鍍金屬氧化物作為電子傳輸層(氧化鋅)與電洞傳輸層(氧化鉬)，成功製作出在2.7V的電壓以及5.5mA的電流時時具有152cd / m2，EQE為2.7% 的全無機鈣鈦礦(CsPbBr3)發光二極體元件，研究採用全無機之製程與方法可提供未來從事相關研究人員參考與應用。

摘要(英)

All-inorganic perovskite has not only good optoelectronic characteristics but great weather resistance, so lots of researches are being conducted on this material full of potential development to enhance optoelectronic devices such as solar cells and light-emitting diode(LED). We choose thermal evaporation likewise, but different from the two common materials used in dual source co-evaporation deposition, we opt for a single source with CsPbBr3 powder, which effectively solves the problem of accurate ratio control of evaporation material when conducting dual source co-evaporation deposition.
First, we prove that after single-source evaporation deposition the thin film’s quality of CsPbBr3 powder is better than the combination powder of CsBr and PbBr2. Then, we try to improve the quality of CsPbBr3 thin film to solve the derivative phase, CsPb2Br5 and Cs4PbBr6.The excessive amount of CsPb2Br5 and Cs4PbBr6 is likely to make the electrical property of thin film decline and affect the efficiency of LED; accordingly, we eliminate the derivative phase in the thin film and improve the quality by adjusting the temperature and timing of heat treatment, which is used in LED.
We used the metal oxides which are easily acquired and less pollutant, after their energy gap being confirmed through the measurement of UPS, are utilized to construct ETL and HTL in LED and then create a totally inorganic LED component. Under 2.7 volts and 5.5mA, the component has a luminance of 152cd/m2 and EQE is 2.7% shown on a luminance meter.
This study improves the manufacturing process by single-source evaporation deposition. Inorganic LED is created with a thin film whose quality is bettered through heat treatment and metal oxides which are easily acquired and less pollutant as the element in ETL and HTL. Most importantly, this is extremely helpful for the development of commercialization in the future.

關鍵字(中)

★ 鈣鈦礦
★ 單源熱蒸鍍
★ 鈣鈦礦薄膜
★ 發光二極體

關鍵字(英)

★ Perovskite
★ Single-source Vacuum Deposition
★ Perovskite Thin Film
★ Light Emitting Diode

論文目次

摘要 i
Abstract ii
致謝 iii
目錄 iv
圖目錄 vi
表目錄 x
第1章緒論 1
1-1 前言 1
1-2 鈣鈦礦介紹 2
1-3 鈣鈦礦材料介紹 3
1-4 鹵化物鈣鈦礦薄膜製造與應用 6
1-4-1 一步溶液旋塗法 6
1-4-2 多步溶液沉積法 6
1-4-3 溶液-蒸鍍混合法 7
1-4-4 雙源共蒸鍍沉積法 8
1-4-5 雙源逐步沉積法 8
1-4-6 單源共蒸鍍沉積法 9
1-5 鈣鈦礦發光二極體的發展 10
1-6 研究動機 25
第2章實驗方法 26
2-1 實驗材料及儀器 26
2-1-1 實驗材料 26
2-1-2 實驗儀器 26
2-2 實驗步驟 28
2-2-1 ITO 導電玻璃基板清洗 28
2-2-2 二氧化鈦(TiO2)緻密層合成與塗佈 28
2-2-3 氧化鋅(ZnO)合成與塗佈 28
2-2-4 CsPbBr3 蒸鍍 28
2-2-5 MoOx 蒸鍍 28
2-2-6 碳膠刮塗 28
2-2-7 LED 元件量測 29
2-3 實驗分析方式 29
2-3-1 XRD 量測方式 29
2-3-2 UV-vis 量測方式 29
2-3-3 SEM量測方式 29
第3章結果與討論 30
3-1 CsPbBr3 粉末與CsBr + PbBr2 混合粉比較 30
3-2 CsPbBr3 薄膜分析 32
3-2-1 CsPbBr3 粉末使用效率 32
3-2-2 CsPbBr3 薄膜熱處理溫度 33
3-2-3 CsPbBr3 薄膜熱處理時間 34
3-3 UPS 分析 36
3-3-1LED 發光元件主動層 36
3-3-2 LED 發光元件電極替換 38
3-3-3 LED 發光元件電子傳輸層改善 38
3-3-4 LED 發光元件電洞傳輸層改善 40
3-4 LED 發光元件改善 42
3-4-1 LED 發光元件主動層厚度改良 42
3-4-2 LED 發光元件電子與電洞的電荷平衡改善 43
3-4-3 LED 發光元件發光面積改善 44
第4章結論 46
參考文獻 47

參考文獻

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指導教授

詹佳樺(Chia-Hua Chan)

審核日期

2021-1-26

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