雙源順序熱蒸鍍全無機混合鹵化物鈣鈦礦藍色發光二極體之研究;The Study of Dual-source Sequential Vacuum Deposition of Inorganic Mixed Halide Perovskite for Blue Light Emitting Diode

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Title:	雙源順序熱蒸鍍全無機混合鹵化物鈣鈦礦藍色發光二極體之研究;The Study of Dual-source Sequential Vacuum Deposition of Inorganic Mixed Halide Perovskite for Blue Light Emitting Diode
Authors:	曲芸萱;CHU, YUN-HSUAN
Contributors:	機械工程學系
Keywords:	鈣鈦礦;雙源順序熱蒸鍍;全無機混合鹵化物;藍色發光二極體;Perovskite;Dual-source Sequential Vacuum Deposition;Inorganic Mixed Halide;Blue Light Emitting Diode
Date:	2022-08-25
Issue Date:	2022-10-04 12:14:48 (UTC+8)
Publisher:	國立中央大學
Abstract:	全無機金屬鹵化物鈣鈦礦材料因其可以透過調整鹵化物成分來調整能帶，進而擁有從深藍光氯化物、綠光溴化物到近紅外光碘化物的不同的發光顏色，所以被廣泛的使用在光電領域中。在 LED 領域中，由高純度的三原色光打造廣色域，其中藍光可以藉由混和 Cl 和 Br 的鹵化物鈣鈦礦實現，但效率及穩定性都大幅落後綠光及紅光 LED，而目前學術上關於蒸鍍製程的研究很少，主流採用溶液法製程製備藍光 LED，並時常加入部份有機離子團(如 MA+、FA+和 PEA+等)來提升性能，並非全無機鈣鈦礦材料。本研究主要是利用雙源順序蒸鍍法以固定厚度比例分別蒸鍍 CsPbCl3 和 CsPbBr3 材料，取代了利用單源熱蒸鍍製程蒸鍍 CsPbBr3-xClx材料，並利用 XRD、UV-vis 及 SEM 展示了雙源順序蒸鍍的優勢，再進一步搭配製程後退火處理製備出具高品質的 CsPbBr3-xClx發光薄膜，其 PL 波長為 463.1nm，FWHM 為 16.2nm。將薄膜應用在 LED 中作為主動層，並經過 UPS 量測分析後確認其能階位置，印證元件以 ITO/ALD-ZnO/CsPbBr3-xClx/碳膠的結構符合能階的匹配。為了使元件亮度等性能得到改善，本研究主要針對主動層的熱處理時間、平整性、結晶性、孔洞缺陷和均勻性進行一系列的改良，最後成功以主動層參數為 CsPbBr3-CsPbCl3-CsPbBr3 的三明治結構，在電壓為 3.9V 以及電流密度為 691mA/cm2 時，得到最大亮度 289nits，在 CIE 1931 色域圖中座標為(0.1363,0.0958)，對應發光波長為 470.4nm。;All-inorganic metal halide perovskite materials are widely used in the field of optoelectronics, because they can adjust the energy band by adjusting the halide composition, and then have different emission colors from deep blue chloride, green bromide to near-infrared iodide. In the field of LED research, a wide color gamut is created from high-purity three primary colors. Among them, blue light emitting layer can be obtained by mixed halide perovskite with Cl and Br, but the efficiency and stability are far behind green and red one. At present, little research about blue and green LED has been conducted in evaporation process. Most of the research is conducted in solution process to prepare blue LEDs, and often use partial organic cation groups(such as MA+ , FA+ and PEA+ ) to improve device performance, which isn’t all-inorganic metal halide perovskite material. In this study, CsPbCl3 and CsPbBr3 powder is evaporated respectively with a fixed thickness ratio by the dual-source sequential vacuum deposition, instead of the single-source vacuum deposition to evaporate the CsPbBr3-xClx powder, and XRD, UV-vis and SEM are used to demonstrate the advantages of dual-source sequential vacuum deposition. The obtained film is further annealed after the deposition process to prepare a high-quality CsPbBr3-xClx lumenescent film with PL wavelength of 463.1 nm and FWHM of 16.2 nm. The CsPbBr3-xClx thin film is applied in the LED as the active layer, and UPS measurement and analysis confirm the energy level position and energy level matching of the LED with the structure of ITO /ALD-ZnO /CsPbBr3-xClx /C. In this study, annealing process, flatness, crystallinity, hole defects and uniformity of the active layer have been improved to enhance LED performance. Finally, the active layer of CsPbBr3-CsPbCl3-CsPbBr3 sandwich structure obtain the maximum luminance of 289nits, CIE coordinate of (0.1363, 0.0958) and the corresponding emission wavelength of 470.4nm at 3.9V and 691mA/cm2 .
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