具有接近单位量子效率的全无机零维 Sn 掺杂 Rb4CdCl6,The Journal of Physical Chemistry C

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具有接近单位量子效率的全无机零维 Sn 掺杂 Rb4CdCl6
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2023-02-13 , DOI: 10.1021/acs.jpcc.2c08483
Jiali Yao ₁ , Chi Cao ₁ , Haiming Cheng ₁ , Dayang Wang ₁ , Wensheng Yang _{1,

2,

3} , Renguo Xie ₁

Affiliation

零维（0D）金属卤化物钙钛矿（MHP）由于其独特的晶体和电子结构而备受关注。与三维 (3D) CsPbCl ₃类似物截然不同，0D 钙钛矿表现出具有大斯托克斯位移和高激子结合能的自陷激子 (STE) 的宽带发射光谱。然而，它们的发光效率远低于 3D 的发光效率。在此，我们首次成功合成了Sn ²⁺掺杂的0D Rb ₄ CdCl ₆通过简单的水热法在 485 nm 发射。重要的是，掺杂 0.239 Sn 的主体在紫外光激发下显示出接近单位的量子效率（PLQY ∼98.04%），这是 Cd 基全无机 MHP 中最高的。依赖于温度的 PL 光谱的结果表明，发射可能源自 STE，其中这种广泛的发射归因于主体基质中八面体 [SnCl ₆ ] ^{4–单元的}³ P ₁到¹ S _{0辐射跃迁。}结果，所制备的掺杂晶体表现出大的斯托克斯位移和高量子效率。我们的工作成功地阐明了 Sn ²⁺掺杂剂在改善 0D MHP 的 PLQY 方面起着不可或缺的作用。这种掺杂Sn ²⁺的有前途的发光材料在光电器件中具有重要的应用前景。

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All-Inorganic Zero-Dimensional Sn-Doped Rb4CdCl6 with Near-Unity Quantum Efficiency

Zero-dimensional (0D) metal halide perovskites (MHPs) have attracted much attention due to their unique crystal and electronic structure. Drastically different from three-dimensional (3D) CsPbCl₃ analogues, 0D perovskites exhibit broadband emission spectra of self-trapped excitons (STEs) with a large Stokes shift and high exciton binding energy. However, their luminescent efficiencies are much lower than those of the 3D ones. Herein, for the first time, we successfully synthesized the Sn²⁺-doped 0D Rb₄CdCl₆ with an emission at 485 nm by a simple hydrothermal method. Importantly, the host with a doping of 0.239 Sn shows a near-unity quantum efficiency (PLQY ∼98.04%) under UV light excitation, which is the highest among Cd-based all-inorganic MHPs. The results from temperature-dependent PL spectra suggested that the emission might originate from STEs, where this broad emission is attributed to the ³P₁ to ¹S₀ radiation transition of octahedral [SnCl₆]^4– units in the host matrix. As a result, the as-prepared doped crystals exhibit large Stokes shifts and high quantum efficiency. Our work successfully elucidates that the Sn²⁺ dopant plays an integral role in improving PLQY of 0D MHPs. This kind of Sn²⁺-doped promising luminescent materials may have significant applications in optoelectronic devices.

更新日期：2023-02-13

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