Zhong Yu, Liu Si-Ping, Lin Yang-Peng, Qi Xing-Hui, Yang Bin, Zhang Qing, Du Ke-Zhao
Fujian Key Laboratory of Polymer Materials, Collage of Chemistry and Material Science, Fujian Normal University, Fuzhou 350007, People's Republic of China.
Qinghai Environmental Monitoring Center, Xining 810000, P. R. China.
Inorg Chem. 2023 Sep 4;62(35):14422-14430. doi: 10.1021/acs.inorgchem.3c02293. Epub 2023 Aug 22.
Metal ion-doped zero-dimensional halide perovskites provide good platforms to generate broadband emission and explore the fundamental dynamics of emission regulations. Recently, Sb-doped zero-dimensional halide perovskites have attracted considerable attention for the high quantum yield of yellow emission; however, the triplet state recombination is activated and the singlet state emission is usually absent. Herein, we fabricate an Sb-doped zero-dimensional [(CH)N]SnCl perovskite that can induce singlet and triplet emission. Density functional theory calculation shows that there are some overlaps between the highest occupied molecular orbitals and the lowest unoccupied molecular orbitals, which may induce a large energy separation between the lowest excited triplet states (T) and the lowest excited singlet states (S) [Δ(S - T)], impeding all the carriers' transfer from the singlet state to the triplet state. As a result, the reserved singlet emission together with the triplet emission can be regulated by excitation wavelength in situ. In addition, different Bi ratios are co-doped into Sb@[(CH)N]SnCl, resulting in a photoluminescence ex situ regulation. Single-phase white light LED and optical anti-counterfeiting are developed further.
金属离子掺杂的零维卤化物钙钛矿为产生宽带发射和探索发射调控的基本动力学提供了良好的平台。最近，锑掺杂的零维卤化物钙钛矿因其黄色发射的高量子产率而备受关注；然而，三重态复合被激活，单重态发射通常不存在。在此，我们制备了一种能诱导单重态和三重态发射的锑掺杂零维[(CH)N]SnCl钙钛矿。密度泛函理论计算表明，最高占据分子轨道和最低未占据分子轨道之间存在一些重叠，这可能导致最低激发三重态（T）和最低激发单重态（S）之间存在较大的能量分离[Δ(S - T)]，阻碍了所有载流子从单重态向三重态的转移。结果，保留的单重态发射与三重态发射可以通过激发波长原位调控。此外，不同的铋比例共掺杂到Sb@[(CH)N]SnCl中，实现了光致发光的异位调控。进一步开发了单相白光发光二极管和光学防伪技术。
