Zhou Bo, Fang Feier, Liu Zexiang, Zhong Haizhe, Zhou Kang, Hu Hanlin, Min Jiacheng, Zheng Fangyuan, Fang Shaofan, Nie Jingheng, Huang Jing-Kai, Li Lain-Jong, Li Henan, Wan Yi, Shi Yumeng
School of Electronics and Information Engineering, Shenzhen University, Shenzhen 518060, China.
International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen 518060, China.
J Am Chem Soc. 2024 Jun 5;146(22):15198-15208. doi: 10.1021/jacs.4c02108. Epub 2024 May 14.
Various monovalent cations are employed to construct metal halide perovskites with various structures and functionalities. However, perovskites based on highly polar A-site cations have seldom been reported. Here, a novel hybrid 0D (NH)(OH)InCl perovskite with highly polar hydronium OH cations is introduced in this study. Upon doping with Sb, hybrid 0D (NH)(OH)InCl single crystals exhibited highly efficient broadband yellowish-green (550 nm) and red (630 nm) dual emissions with a PLQY of 86%. The dual emission arises due to Sb occupying two sites within the crystal lattice that possess different polarization environments, leading to distinct Stokes shift energies. The study revealed that lattice polarity plays a significant role in the self-trapped exciton emission of Sb-doped perovskites, contributing up to 25% of the Stokes shift energy for hybrid 0D (NH)(OH)InCl:Sb as a secondary source, in addition to the Jahn-Teller deformation. These findings highlight the potential of Sb-doped perovskites for achieving tunable broadband emission and underscore the importance of lattice polarity in determining the emission properties of perovskite materials.
各种单价阳离子被用于构建具有不同结构和功能的金属卤化物钙钛矿。然而，基于高极性A位阳离子的钙钛矿鲜有报道。在此，本研究引入了一种具有高极性水合氢离子OH阳离子的新型混合0D (NH)(OH)InCl钙钛矿。在用Sb掺杂后，混合0D (NH)(OH)InCl单晶表现出高效的宽带黄绿色（550 nm）和红色（630 nm）双发射，其光致发光量子产率为86%。这种双发射是由于Sb占据了晶格内两个具有不同极化环境的位置，导致了不同的斯托克斯位移能量。该研究表明，晶格极性在掺Sb钙钛矿的自陷激子发射中起着重要作用，除了 Jahn-Teller 变形外，还作为次要来源为混合0D (NH)(OH)InCl:Sb贡献了高达25%的斯托克斯位移能量。这些发现突出了掺Sb钙钛矿实现可调谐宽带发射的潜力，并强调了晶格极性在决定钙钛矿材料发射特性方面的重要性。
