Structural Transformation and Photoluminescent Property of Manganese-Doped Bismuth-Based Perovskites,Inorganic Chemistry

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Structural Transformation and Photoluminescent Property of Manganese-Doped Bismuth-Based Perovskites
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2023-06-01 , DOI: 10.1021/acs.inorgchem.3c00957
Jing Liu ₁ , Qichuan Hu ₁ , Hailong Yu ₁ , Hanqi Xu ₁ , Jinyang Yu ₁ , Qiuju Han ₂ , Wenzhi Wu ₁

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Here, we synthesized pure Cs₃Bi₂Cl₉ (CBC) and manganese (Mn)-doped crystals with different feeding ratios, leading to changes in structure and luminescence. The crystals Cs₃Bi₂Cl₉–Mn (CBCM) formed by doping a minor amount of Mn²⁺ (Bi/Mn = 8:1) maintain the orthorhombic phase structure of the host, but when Bi/Mn = 2:1, the crystal structure is more inclined to form Cs₄MnBi₂Cl₁₂ (CMBC) of a trigonal phase. Combined with density functional theory (DFT) calculation, the results demonstrate that a moderate amount of Mn²⁺ doping can create impurity energy levels in the forbidden band. However, as the structure transitions, the type of energy band structure changes from indirect to direct, with completely different electronic orbital features. Temperature-dependent time-resolved and steady-state photoluminescence spectroscopies are used to explore the structure-related thermal properties and transitional process. Differences energy transfer routes are revealed, with CBCM relying on intersystem energy transfer and CMBC mainly depending on direct excitation of Mn²⁺ to produce d–d transitions. Furthermore, since CMBC is temperature-sensitive, we perform the first photoluminescent (PL) lifetime temperature measurement using CBMC and obtain a maximum relative sensitivity of 1.7 %K^–1 and an absolute sensitivity of 0.0099 K^–1. Our work provides insight into the mechanism of Mn²⁺ doping-induced luminescence and offers a potentially effective doping strategy for improving the PL properties of lead-free metal halide perovskites.

中文翻译：

锰掺杂铋基钙钛矿的结构转变和光致发光性能

在这里，我们合成了具有不同进料比的纯 Cs ₃ Bi ₂ Cl ₉ (CBC) 和锰 (Mn) 掺杂晶体，导致结构和发光发生变化。通过掺杂少量 Mn ²⁺ (Bi/Mn = 8:1) 形成的晶体 Cs ₃ Bi ₂ Cl ₉ –Mn ( CBCM) 保持主体的正交相结构，但当 Bi/Mn = 2:1 时，晶体结构更倾向于形成三方相的Cs ₄ MnBi ₂ Cl _{12 (CMBC)。}结合密度泛函理论（DFT）计算，结果表明适量的Mn ²⁺掺杂可以在禁带中产生杂质能级。然而，随着结构的转变，能带结构类型从间接变为直接，具有完全不同的电子轨道特征。温度相关的时间分辨和稳态光致发光光谱用于探索与结构相关的热性质和过渡过程。揭示了不同的能量传递途径，CBCM 依赖于系间能量传递，而 CMBC 主要依赖于 Mn ²⁺的直接激发产生 d-d 跃迁。^{此外，由于 CMBC 对温度敏感，我们使用 CBMC 进行了第一次光致发光 (PL) 寿命温度测量，并获得了 1.7 %K –1}的最大相对灵敏度^{以及 0.0099 K –1}的绝对灵敏度。^{我们的工作提供了对 Mn 2+}掺杂诱导发光机制的深入了解，并提供了一种潜在有效的掺杂策略来改善无铅金属卤化物钙钛矿的 PL 性能。

更新日期：2023-06-01

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