The Role of Halogen Atoms on High-Efficiency Mn2+ Emission in Two-Dimensional Hybrid Perovskites.
The Role of Halogen Atoms on High-Efficiency Mn2+ Emission in Two-Dimensional Hybrid Perovskites.
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DOI：
10.1021/acs.jpclett.9b01996
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发表时间：
2019-07
期刊：
影响因子：
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通讯作者：
Guojun Zhou;X. Jia;Shaoqiang Guo;M. Molokeev;Junying Zhang;Z. Xia
中科院分区：
文献类型：
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作者：
Guojun Zhou;X. Jia;Shaoqiang Guo;M. Molokeev;Junying Zhang;Z. Xia
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能的影响仍然是一个挑战。在此，确定了二维杂化钙钛矿 BA2PbX4 (BA = C4H9NH3) 中 X 成分对掺杂 Mn2+ 发射的作用，其中 Mn2+ 显示出对卤素性质的强烈发光依赖性，并且在 BA2PbBr4 中实现了最佳 Mn2+ 发射，其量子产率为创纪录的 60.1%。密度泛函理论计算表明，BA2PbBr4 具有较低的 Br 空位浓度，并且在导带最小值处具有独特的 Mn-3d 能级和 Pb-6p 能级耦合态，从而实现从主体到 Mn2+ 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。
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-dimentional hybrid perovskite BA2PbX4 (BA = C4H9NH3) on the doped Mn2+ emission is identified, wherein Mn2+ reveals a strong luminescence dependence on the nature of the halogen, and optimum Mn2+ emission with the record quantum yield of 60.1% has been achieved in BA2PbBr4. Density functional theory calculations show that BA2PbBr4 holds low Br vacancy concentration, and unique coupled states of Mn-3d level and Pb-6p level at the conduction band minimum, leading to the efficient energy transfer from host to Mn2+. Our work sheds new lights on the methods to realize strong exciton-dopant exchange coupling for achieving high-efficiency dopant luminescence.