The mechanochemical route is a facile and fast way and has received much attention for developing versatile advanced functional materials. Herein, we reported a mechanochemical synthesis for incorporating divalent man...The mechanochemical route is a facile and fast way and has received much attention for developing versatile advanced functional materials. Herein, we reported a mechanochemical synthesis for incorporating divalent manganese ions (Mn^Ⅱ) into a two-dimensional (2D) hybrid perovskite (C4H9NH3)2PbCl4. The mild external stimuli originating from the grinding at room temperature enabled the formation of Mn^Ⅱ-doped 2D hybrid perovskites, and rapidly changed the luminescence characteristics. The photoluminescence analyses show that the violet and orange emissions are attributed to (C4H9NH3)2Pb1-xMnxCl4 band-edge emission and the T1→^6A1 transition of Mn^2+ resulting from an efficient energy transfer process, respectively. Site preference and distribution of the doped Mn^2+ cations on the locations of Pb^2+ were analyzed. The formation energy calculated by the density functional theory (DFT) indicates that the Mn^2+ ions can rapidly enter the crystal lattice due to the unique 2D crystal structure of the hybrid perovskite. Such a case of mechanochemical synthesis for the 2D hybrid perovskite motivates many novel emerging materials and the related applications.展开更多
基金supported by the National Natural Science Foundation of China (91622125, 51722202 and 51572023)the Natural Science Foundation of Beijing (2172036)the support of the Russian Foundation for Basic Research (17-52-53031)
文摘The mechanochemical route is a facile and fast way and has received much attention for developing versatile advanced functional materials. Herein, we reported a mechanochemical synthesis for incorporating divalent manganese ions (Mn^Ⅱ) into a two-dimensional (2D) hybrid perovskite (C4H9NH3)2PbCl4. The mild external stimuli originating from the grinding at room temperature enabled the formation of Mn^Ⅱ-doped 2D hybrid perovskites, and rapidly changed the luminescence characteristics. The photoluminescence analyses show that the violet and orange emissions are attributed to (C4H9NH3)2Pb1-xMnxCl4 band-edge emission and the T1→^6A1 transition of Mn^2+ resulting from an efficient energy transfer process, respectively. Site preference and distribution of the doped Mn^2+ cations on the locations of Pb^2+ were analyzed. The formation energy calculated by the density functional theory (DFT) indicates that the Mn^2+ ions can rapidly enter the crystal lattice due to the unique 2D crystal structure of the hybrid perovskite. Such a case of mechanochemical synthesis for the 2D hybrid perovskite motivates many novel emerging materials and the related applications.