Zeng Ruosheng, Zhang Leilei, Xue Yang, Ke Bao, Zhao Zhuang, Huang Dan, Wei Qilin, Zhou Weichang, Zou Bingsuo
School of Materials Science and Engineering, School of Life and Environmental Sciences, Guilin University of Electronic Technology, Guilin 541004, People's Republic of China.
School of Physical Science and Technology, Key Laboratory of New Processing Technology for Non-ferrous Metals and Materials (Ministry of Education), Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials, Guangxi University, Nanning 530004, People's Republic of China.
J Phys Chem Lett. 2020 Mar 19;11(6):2053-2061. doi: 10.1021/acs.jpclett.0c00330. Epub 2020 Feb 28.
Highly efficient blue-emitting three-dimensional (3D) lead-free halide perovskites with excellent stability have attracted worldwide attention. Herein, a doping route was adopted to incorporate Sb ions into the CsNaInCl for decorating the electronic band structure. Due to the moderate electron-phonon coupling, the Sb-doped CsNaInCl double perovskites showed a narrow and relatively unusual blue emission of self-trapped excitons (STEs). Density functional theory (DFT) calculation indicated that the doped Sb ions could break the parity-forbidden transition rule and modulate the density of state (DOS) population effectively to boost the PLQY of STEs drastically. The optimized Sb:CsNaInCl exhibited a PLQY of up to 75.89% and excellent stability under the consecutive illumination of 365 nm UV light for 1000 h. This kind of highly efficient lead-free Sb-doped CsNaInCl double perovskites may overcome the bottlenecks of severe toxicity and insufficient stability and therefore have an extensive application in the scarce blue photonic and optoelectronic fields.
具有优异稳定性的高效蓝色发光三维（3D）无铅卤化物钙钛矿引起了全球关注。在此，采用掺杂路线将Sb离子引入CsNaInCl中以修饰电子能带结构。由于适度的电子-声子耦合，Sb掺杂的CsNaInCl双钙钛矿表现出自陷激子（STE）的窄且相对不寻常的蓝色发射。密度泛函理论（DFT）计算表明，掺杂的Sb离子可以打破宇称禁戒跃迁规则并有效调节态密度（DOS）分布，从而大幅提高STE的光致发光量子产率（PLQY）。优化后的Sb:CsNaInCl在365 nm紫外光连续照射1千小时下表现出高达75.89%的PLQY和优异的稳定性。这种高效的无铅Sb掺杂CsNaInCl双钙钛矿可能克服严重毒性和稳定性不足的瓶颈，因此在稀缺的蓝色光子和光电子领域具有广泛应用。
