Zhou Guojun, Jia Xiaofang, Guo Shaoqiang, Molokeev Maxim, Zhang Junying, Xia Zhiguo
The Beijing Municipal Key Laboratory of New Energy Materials and Technologies School of Materials Sciences and Engineering , University of Science and Technology Beijing , Beijing 100083 , China.
Key Laboratory of Micro-Nano Measurement, Manipulation and Physics (Ministry of Education), School of Physics , Beihang University , Beijing 100191 , China.
J Phys Chem Lett. 2019 Aug 15;10(16):4706-4712. doi: 10.1021/acs.jpclett.9b01996. Epub 2019 Aug 6.
Doped halide pervoskites as highly efficient light emitters have recently fascinated the research community, while the influence of halogen atoms X (X = Cl, Br, I) on the hybrid energy levels and photoluminescence properties remains a challenge. Here, the role of X compositions in the two-dimensional hybrid perovskite BAPbX (BA = CHNH) on the doped Mn emission is identified, wherein Mn reveals a strong luminescence dependence on the nature of the halogen, and optimum Mn emission with a record quantum yield of 60.1% has been achieved in BAPbBr. Density functional theory calculations show that BAPbBr holds low Br vacancy concentration and unique coupled states of the Mn-3d level and Pb-6p level at the conduction band minimum, leading to efficient energy transfer from the host to Mn. Our work sheds new light on the methods to realize strong exciton-dopant exchange coupling for achieving high-efficiency dopant luminescence.
掺杂卤化物钙钛矿作为高效发光体最近引起了研究界的关注，而卤素原子X（X = Cl、Br、I）对混合能级和光致发光性质的影响仍然是一个挑战。在此，确定了二维混合钙钛矿BAPbX（BA = CHNH）中X组成对掺杂Mn发射的作用，其中Mn的发光强烈依赖于卤素的性质，并且在BAPbBr中实现了创纪录的60.1%量子产率的最佳Mn发射。密度泛函理论计算表明，BAPbBr具有低Br空位浓度以及在导带最小值处Mn-3d能级和Pb-6p能级的独特耦合态，从而导致从主体到Mn的有效能量转移。我们的工作为实现强激子-掺杂剂交换耦合以实现高效掺杂剂发光的方法提供了新的思路。
