Peng Yu, Li Lina, Ji Chengmin, Wu Zhenyue, Wang Sasa, Liu Xitao, Yao Yunpeng, Luo Junhua
State Key Laboratory of Structural Chemistry , Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences , Fuzhou , Fujian 350002 , P. R. China.
School of Physical Science and Technology , ShanghaiTech University , Shanghai 201210 , China.
J Am Chem Soc. 2019 Aug 7;141(31):12197-12201. doi: 10.1021/jacs.9b04829. Epub 2019 Jul 30.
Organic-inorganic lead halide hybrids have attracted extensive interest in solid-state lighting, due to their superior color tunability and low-cost solution processing. However, the relatively low photoluminescence quantum efficiency (PLQE) is a common issue for most bulk lead halide hybrids. Inspired by the intriguing luminescence properties of heterometallic complexes, we rationally developed an unprecedented two-dimensional (2D) Pb-Mn heterometallic halide hybrid, (CHN)PbMnCl (), through a precisely tailored synthetic approach based on (CHN)PbCl (). Intriguingly, features a unique 2D heterometallic halide layer configuration, in which the strong quantum confinement facilitates efficient energy transfer from bound excitons to d-states of Mn, resulting in highly sensitized Mnemission. The PLQE of is up to 32%, considerably higher than that of pristine (less than 1%). Moreover, presents significant environmental and thermal stability, benefiting from its cluster feature. To our best knowledge, this is the first example of construction of a Pb-Mn heterometallic halide hybrid with bulk highly efficient red emission. This work provides a way to enhance the PLQE of lead halide hybrids via sensitization in rationally designed heterometallic halide hybrids.
有机-无机卤化铅杂化物因其出色的颜色可调性和低成本溶液加工工艺而在固态照明领域引起了广泛关注。然而，相对较低的光致发光量子效率（PLQE）是大多数块状卤化铅杂化物普遍存在的问题。受异金属配合物有趣发光特性的启发，我们基于(CHN)PbCl()通过精确定制的合成方法合理开发了一种前所未有的二维（2D）Pb-Mn异金属卤化物杂化物(CHN)PbMnCl()。有趣的是，其具有独特的二维异金属卤化物层结构，其中强大的量子限域效应促进了从束缚激子到Mn的d态的有效能量转移，从而产生高度敏化的Mn发射。的PLQE高达32%，远高于原始的（小于1%）。此外，由于其簇状特征，具有显著的环境和热稳定性。据我们所知，这是构建具有块状高效红色发射的Pb-Mn异金属卤化物杂化物的首个例子。这项工作提供了一种通过在合理设计的异金属卤化物杂化物中进行敏化来提高卤化铅杂化物PLQE的方法。
