Yue Cheng-Yang, Sun Chen, Li Dong-Yang, Dong Yu-Han, Wang Chun-Lei, Zhao Hui-Fang, Jiang Hao, Jing Zhi-Hong, Lei Xiao-Wu
Department of Chemistry and Chemical Engineering , Jining University , Qufu , Shandong 273155 , P. R. China.
College of Chemistry and Chemical Engineering , Qufu Normal University , Qufu , Shandong 273165 , P. R. China.
Inorg Chem. 2019 Aug 5;58(15):10304-10312. doi: 10.1021/acs.inorgchem.9b01472. Epub 2019 Jul 22.
In recent years, although low-dimensional hybrid lead halides have received great attention due to the fascinating photoluminescent (PL) properties, the research is still on the early stage and only limited phases have been explored and characterized. Here, by introducing heterometals as mixed structural compositions and optical activity centers, we prepared a series of low-dimensional hybrid heterometallic halides, namely as, [(Me)-DABCO]CuPbI, [(Me)-DABCO]MPbI (M = Cu and Ag) and [(Me)-DABCO]AgPbBr (Me = methyl group, DABCO = 1,4-diazabicyclo[2.2.2]octane). These hybrid halides feature a low-dimensional 0D [CuPbI] cluster, a 1D [MPbI] chain, and a 2D [AgPbBr] layer, respectively, on the basis of corner-, edge- and face-sharing connecting of [MX] tetrahedrons, [PbX] quadrangular pyramids, and [PbX] octahedrons. Under the photoexcitation, these hybrid heterometallic halides exhibit deep-red luminescent emissions from 711 to 801 nm with the largest Stocks shift of 395 nm. The temperature-dependent PL emissions, PL lifetime, and theoretical calculations are also investigated to probe into the intrinsic nature of photoluminescent emissions. This work affords new types of hybrid halides by introducing different metal centers to probe into the structural evolution and photoluminescent properties.
近年来，尽管低维混合铅卤化物因其迷人的光致发光（PL）特性而备受关注，但研究仍处于早期阶段，仅探索和表征了有限的物相。在此，通过引入异金属作为混合结构组成和光学活性中心，我们制备了一系列低维混合异金属卤化物，即[(Me)-DABCO]CuPbI、[(Me)-DABCO]MPbI（M = Cu和Ag）以及[(Me)-DABCO]AgPbBr（Me = 甲基，DABCO = 1,4 - 二氮杂双环[2.2.2]辛烷）。这些混合卤化物分别基于[MX]四面体、[PbX]四角锥和[PbX]八面体的角共享、边共享和面共享连接，具有低维的0D [CuPbI]簇、1D [MPbI]链和2D [AgPbBr]层。在光激发下，这些混合异金属卤化物在711至801 nm处呈现深红色发光发射，最大斯托克斯位移为395 nm。还研究了温度依赖的PL发射、PL寿命和理论计算，以探究光致发光发射的内在本质。这项工作通过引入不同的金属中心提供了新型混合卤化物，以探究结构演变和光致发光特性。
