嵌入 Cs4PbBr6 晶体中的光致发光纳米 CsPbBr3：形成机制和性能,Crystal Growth & Design

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嵌入 Cs4PbBr6 晶体中的光致发光纳米 CsPbBr3：形成机制和性能
Crystal Growth & Design ( IF 3.2 ) Pub Date : 2023-12-16 , DOI: 10.1021/acs.cgd.3c01226
Weihao Sun, Yuan-Ting Hung, Wen-Tse Huang, Ru-Shi Liu, Wuzong Zhou

采用反溶剂法合成了发光晶体溴化铯铅，前驱体中 Cs:Pb 的标称比在 4.5:1 至 1:1 范围内变化。尽管所有样品的粉末X射线衍射图均显示Cs ₄ PbBr ₆为纯相或主相，但高分辨率透射电子显微镜图像显示，所有Cs ₄ PbBr ₆晶体中均嵌入有大量CsPbBr ₃纳米微晶。。提出了这些钙钛矿纳米微晶作为光致发光实际活性中心的形成机制。^{晶体生长中最关键的步骤是沉积含有通过 Cs +}连接的聚合 PbBr ₆^4–的非晶涂层，Cs:Pb 比例约为 3:1，因此，实际的晶体生长位点位于界面处晶体和涂层之间，而不是晶体/溶液界面。_{Cs 4} PbBr ₆形成过程中局部缺乏Cs导致在Cs ₄ PbBr ₆母晶体内部形成CsPbBr ₃纳米微晶。与裸露的CsPbBr 3 晶体相比，_{嵌入的CsPbBr 3}_纳米晶的光致发光量子产率和稳定性显着提高。母体晶体和嵌入的纳米微晶的这种同时生长为铯铅卤化物基光致发光材料的进一步开发提供了线索。

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Photoluminescent Nano-CsPbBr3 Embedded in Cs4PbBr6 Crystals: Formation Mechanism and Properties

Luminescent crystalline cesium lead bromide has been synthesized by using an antisolvent method with the nominal ratio of Cs:Pb in the precursors varying in a wide range from 4.5:1 to 1:1. Although the powder X-ray diffraction patterns of all the specimens show Cs₄PbBr₆ as a pure phase or a main phase, high-resolution transmission electron microscopy images reveal a large amount of CsPbBr₃ nanocrystallites embedded in all the Cs₄PbBr₆ crystals. A formation mechanism of these perovskite nanocrystallites serving as actual active centers of photoluminescence is proposed. The most crucial step in the crystal growth is the deposition of a noncrystalline coating layer containing polymerized PbBr₆^4– linked by Cs⁺ with the Cs:Pb ratio of about 3:1, and therefore, the actual crystal growth sites are at the interface between the crystal and the coating layer, instead of the crystal/solution interface. The local lack of Cs during the formation of Cs₄PbBr₆ results in the formation of CsPbBr₃ nanocrystallites inside the parent crystals of Cs₄PbBr₆. The photoluminescence quantum yield and stability of the embedded CsPbBr₃ nanocrystallites are significantly improved in comparison with bare CsPbBr₃ crystals. Such simultaneous growth of parent crystals and the embedded nanocrystallites sheds light on further development of cesium lead halide-based photoluminescent materials.

更新日期：2023-12-16

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