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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题名:	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
作者:	葉冠奇;Yeh, Kuan-Chi
贡献者:	能源工程研究所
关键词:	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;Single-Source Vapor Deposition;Heat Treatment;Perovskite CsPbBr3;CsPbBr3 Light-Emitting Diodes;CsPbBr3 Photoluminescence Films
日期:	2025-01-16
上传时间:	2025-04-09 17:21:12 (UTC+8)
出版者:	國立中央大學
摘要:	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。;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.
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