Li Zhilin, Li Qiaoqiao, Cao Mengyan, Rao Zhihui, Shi Xinyu, Zhou Liujiang, Zhao Xiujian, Gong Xiao
State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China.
Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou 313001, China.
Langmuir. 2023 Mar 14;39(10):3792-3799. doi: 10.1021/acs.langmuir.3c00129. Epub 2023 Feb 28.
Low-dimension perovskite materials have attracted wide attention due to their excellent optical properties and stability. Herein, Sb-doped CsZrCl crystals are synthesized by a coprecipitation method in which Sb ions partially replace Zr ions. The CsZrCl:Sb powder shows blue and orange-red emissions under a 254 and 365 nm light, respectively, due to the [ZrCl] octahedron and [SbCl] octahedron. The photoluminescence quantum yield (PLQY) of CsZrCl:Sb ( = 0.1) crystals is up to 52.5%. According to experimental and computational results, the emission mechanism of the CsZrCl:Sb crystals is proposed. On the one hand, a wide blue emission with a large Stokes shift is caused by the self-trapping excitons of [ZrCl] octahedra under a 260 nm excitation. On the other hand, the luminescence mechanism of [SbCl] octahedron is divided into two parts: P → S (490 nm) and P → S (625 nm). The broad-band emission, high PLQY, and excellent stability endow the CsZrCl:Sb powders with the potential for the fabrication of white light-emitting diodes (WLEDs). A WLED device is fabricated using a commercial 310 nm NUV chip, which shows a high color rendering index of 89.7 and a correlated color temperature of 5333 K. In addition, the synthesized CsZrCl:Sb crystals can be also successfully used for information encryption. Our work will provide a deep understanding of the photophysical properties of Sb-doped perovskites and facilitate the development of CsZrCl:Sb crystals in encrypting multilevel optical codes and WLEDs.
低维钙钛矿材料因其优异的光学性能和稳定性而受到广泛关注。在此,通过共沉淀法合成了Sb掺杂的CsZrCl晶体,其中Sb离子部分取代Zr离子。由于[ZrCl]八面体和[SbCl]八面体,CsZrCl:Sb粉末在254和365 nm光下分别呈现蓝色和橙红色发射。CsZrCl:Sb( = 0.1)晶体的光致发光量子产率(PLQY)高达52.5%。根据实验和计算结果,提出了CsZrCl:Sb晶体的发射机制。一方面,在260 nm激发下,[ZrCl]八面体的自陷激子导致了具有大斯托克斯位移的宽蓝色发射。另一方面,[SbCl]八面体的发光机制分为两部分:P → S(490 nm)和P → S(625 nm)。宽带发射、高PLQY和优异的稳定性赋予了CsZrCl:Sb粉末用于制造白光发光二极管(WLED)的潜力。使用商用310 nm近紫外芯片制造了一个WLED器件,其显色指数高达89.7,相关色温为5333 K。此外,合成的CsZrCl:Sb晶体还可成功用于信息加密。我们的工作将深入了解Sb掺杂钙钛矿的光物理性质,并促进CsZrCl:Sb晶体在加密多级光学码和WLED方面的发展。