結合單源氣相沉積與熱處理製程製備高品質全無機鈣鈦礦CsPbBr3光致發光薄膜暨發光二極體之研究

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葉冠奇(Kuan-Chi Yeh) 查詢紙本館藏

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論文名稱

結合單源氣相沉積與熱處理製程製備高品質全無機鈣鈦礦CsPbBr3光致發光薄膜暨發光二極體之研究
(The Study of Fabricating High-Quality All-Inorganic Perovskite CsPbBr3 Photoluminescence Films and Light-Emitting Diodes via Single-Source Vapor Deposition Combined with Heat Treatment)

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至系統瀏覽論文 (2028-2-1以後開放)

摘要(中)

鈣鈦礦材料憑藉卓越的光致發光效率、優異的色純度及低廉的製造成本，在照明與顯示領域展現出巨大潛力。本研究聚焦於CsPbBr3全無機綠光鈣鈦礦薄膜(Perovskite Film, PeFilm)的製備，透過單源氣相沉積(Single Source Vapor Deposition, SSVD)及結合熱退火處理製備高品質CsPbBr3薄膜，以及優化CsPbBr3鈣鈦礦發光二極體(Perovskite Light-Emitting Diode, PeLED)的結構，以提升PeLED發光效率。
通過SSVD 製備的CsPbBr3 PeFilm，在適當熱退火處理後成功從單斜晶相轉變為立方晶相並消除CsPbBr3的異質結構，此過程促進奧斯華擾化效應使晶粒生長與融合更加完整，顯著增強輻射復合能力。研究結果顯示光致發光量子產率 (Photoluminescence Quantum Yield, PLQY)從2.3%提升至52.1%，即使在大氣環境下存放100天PLQY仍能保持在52%以上，展現出卓越的穩定性。此外，將此PeFilm應用於未添加電子與電洞傳輸層的簡單結構PeLED中，元件在2.92 V的操作電壓下達到14,079 cd/m2的最高亮度。
在PeLED結構設計方面為了有效提升元件性能，本研究採用原子層沉積方式製備電子傳輸層ZnO以改善電子傳輸能力。同時，通過交替沉積CsBr與CsPbBr3製備發光層，使其產生具有寬能隙的Cs4PbBr6並形成類量子阱結構，有效限制載子移動並提升輻射復合效率。最終，性能最佳的PeLED在操作電壓2.78 V下最高亮度達到46,812 cd/m2、電流效率達到10.39 cd/A與4.10%的外部量子效率，而且相較於簡單結構的PeLED亮度提升了2.3倍。此外，經30天的大氣環境下進行耐候性測試元件仍能保持原始亮度的60%。值得注意的是，本研究製作的綠光PeLED僅需兩顆市售1.5 V電池即可啟動並達到最高亮度，成功克服普遍PeLED操作電壓偏高的問題，展現出良好的可行性與實用性，為PeLED的發展提供嶄新的製程方式。

摘要(英)

Perovskite materials exhibit excellent photoluminescence efficiency, superior color purity, and low manufacturing cost, demonstrating significant potential in the fields of lighting and display technology. This study focuses on fabricating all-inorganic green-light CsPbBr3 perovskite film (PeFilm) using Single-Source Vapor Deposition (SSVD) combined with thermal annealing to produce high-quality CsPbBr3 films, and optimizing the structure of CsPbBr3 perovskite light-emitting diodes (PeLED) to enhance luminous efficiency.
CsPbBr3 PeFilms fabricated via SSVD successfully transitioned from the monoclinic to the cubic crystalline phase after appropriate thermal annealing, eliminating heterostructures within the CsPbBr3 material. The process facilitated the Ostwald ripening effect, promoting more complete grain growth and fusion, which significantly enhanced radiative recombination efficiency. The study results showed that the photoluminescence quantum yield (PLQY) increased from 2.3% to 52.1%, and even after being stored in an air ambient environment for 100 days, the PLQY remained above 52%, demonstrating exceptional stability. Furthermore, when this PeFilm was applied in a simple PeLEDs structure without additional electron and hole transport layers, the device achieved a maximum brightness of 14,079 cd/m2 at a driving voltage of 2.92 V.
In the design of the PeLED structure, this study utilizes atomic layer deposition to fabricate a ZnO electron transport layer, enhancing electron transport capabilities. The emitting layer is also prepared by alternately depositing CsBr and CsPbBr3, forming a wide bandgap between Cs4PbBr6 and quantum well-like structure, effectively restricting carrier movement and improving radiation recombination efficiency. The optimized PeLED achieved a maximum brightness of 46,812 cd/m2, a current efficiency of 10.39 cd/A, and an external quantum efficiency of 4.10% at an operating voltage of 2.78 V, with Additionally, its brightness was 2.3 times higher compared to PeLEDs with a simpler structure. After 30 days of atmospheric durability testing, the device maintained 60% of its initial brightness. Notably, the green PeLED fabricated in this study can be powered by just two commercially available 1.5 V batteries to achieve its maximum brightness, successfully overcoming the common issue of high driving voltages in PeLEDs, and demonstrating excellent feasibility and practicality. It provides a novel manufacturing approach for advancing PeLED development.

關鍵字(中)

★ 單源氣相沉積
★ 熱處理
★ 鈣鈦礦CsPbBr3
★ CsPbBr3 發光二極體
★ CsPbBr3 光致發光薄膜

關鍵字(英)

★ Single-Source Vapor Deposition
★ Heat Treatment
★ Perovskite CsPbBr3
★ CsPbBr3 Light-Emitting Diodes
★ CsPbBr3 Photoluminescence Films

論文目次

摘要 i
Abstract ii
誌謝 iv
目錄 v
圖目錄 vii
表目錄 xiii
第1章研究背景 1
1-1 鈣鈦礦材料介紹與分類 2
1-1-1 有機-無機鹵化物鈣鈦礦 3
1-1-2全無機鹵化物鈣鈦礦 5
1-2 鈣鈦礦材料在顯示技術應用 8
1-2-1 鈣鈦礦彩色濾光片 8
1-2-2 CsPbBr3 PeLED 11
1-3 溶液法製備PeFilm及應用 15
1-3-1 旋轉塗佈法 16
1-3-2噴墨列印法 18
1-3-3刮塗法 20
1-4蒸鍍法製備PeFilm及應用 22
1-4-1 雙源與多源共蒸鍍法 22
1-4-2 逐步蒸鍍法 24
1-4-3 單源蒸鍍法 26
1-5 熱退火改善PeFilm 28
1-6 CsPbBr3 PeLED的結構組成 30
1-6-1 PeLED之發光層 30
1-6-2 PeLED之電子傳輸層 36
1-6-3 PeLED之電洞傳輸層 38
1-7 研究動機與目的 43
第2章實驗方法 44
2-1 實驗材料及儀器 44
2-1-1 實驗材料 44
2-1-2 實驗儀器 44
2-2 實驗步驟 46
2-2-1 玻璃與ITO基板清洗 46
2-2-2原子層沉積ZnO電子傳輸層 47
2-2-3蒸鍍鈣鈦礦 CsPbBr3發光層 47
2-2-4 發光層熱退火處理 47
2-2-5 碳膠電極刮塗 48
2-2-6 PeLED元件量測 48
2-3 本研究儀器分析方式 48
2-3-1 UV-vis分析及量測方式 48
2-3-2 XRD分析及量測方式 48
2-3-3 SEM分析及量測方式 48
2-3-4 UPS分析及量測方式 49
2-3-5 HR-TEM分析及量測方式 49
2-3-6 積分球與光譜儀分析及量測方式 49
2-3-7 輝度計分析及量測方式 49
第3章利用SSVD 製備CsPbBr3 PeFilm之研究 50
3-1 CsBr/PbBr2混合粉末與CsPbBr3粉末比較 51
3-2熱退火製程提升CsPbBr3薄膜結晶品質 56
3-3 PeFilm的PL和耐候性分析 61
第4章簡單結構CsPbBr3 PeLED之研究 65
4-1熱退火對CsPbBr3 發光層的分析 66
4-2熱退火處理後的CsPbBr3薄膜形貌及功函數分析 71
4-3熱退火製程對 CsPbBr3 PeLED性能的影響 75
第5章發光層及ETL厚度對PeLED效率之研究 79
5-1不同厚度CsPbBr3發光層分析 80
5-2 PeLED的發光層厚度對電流-電壓-亮度性能的影響 82
5-3 利用ALD製備ETL ZnO薄膜探討與分析 85
5-4不同循環次數的ZnO ETL對PeLED性能影響 90
第6章類量子阱結構發光層之PeLED 93
6-1 透過類量子阱結構改善CsPbBr3 PeLED元件性能 94
6-2 不同對數的CsBr+CsPbBr3複合薄膜分析 96
6-3 複合薄膜熱處理前後的微觀變化 103
6-4 不同對數發光層的PeLED性能 107
第7章結論 114
參考文獻 117
發表文獻 131

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指導教授

詹佳樺(Chia-Hua Chan)

審核日期

2025-1-16

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