Deng Zhihao, Ma Junhao, Peng Yuqi, Yao Yuan, Chang Yuanyuan, Qin Nan, Jia Jie, He Rongxing, Zhou Lei, Li Ming
Key Laboratory of Luminescence Analysis and Molecular Sensing (Southwest University), Ministry of Education, Chongqing Key Laboratory of Soft-Matter Material Chemistry and Function Manufacturing, School of Chemistry and Chemical Engineering, Southwest University, Chongqing 400715, China.
Institute of Materials Science and Devices, School of Materials Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009 , P. R. China.
Inorg Chem. 2025 Mar 3;64(8):4103-4112. doi: 10.1021/acs.inorgchem.4c05549. Epub 2025 Feb 14.
Organic-inorganic hybrid Sn(IV)-based metal halides have received wide attention due to their excellent structural stability. However, realizing red-emitting Sn(IV)-based metal halides with high stability and efficient photoluminescence (PL) efficiency remains challenging. Here, a stable organic-inorganic Sn(IV)-based metal halide (CHON)SnCl with a zero-dimensional (0D) structure has been obtained, which, however, displays poor PL properties due to the inert expression of Sn-4d electrons and the intrinsic indirect band gap feature. To address the above challenges, Te with an active 5s lone pair is embedded into the lattice of (CHON)SnCl, and as a result, 5%Te-doped (CHON)SnCl with a direct band gap exhibits a broadband deep-red emission (∼688 nm) with a high PL efficiency (∼53%). Experimental and calculated results reveal that the embedding of Te can effectively regulate the band structure of (CHON)SnCl to facilitate the transformation from an indirect to a direct band structure, thereby leading to efficient radiative recombination. Benefiting from the above merits, a high-efficiency white light-emitting diode (WLED) has been fabricated using Te-doped (CHON)SnCl with an ultrahigh color rendering index (CRI) of up to 94.5, suggesting the great potential of this material for solid-state lighting. This work provides significant insight into the design of highly efficient red-emitting phosphors for organic-inorganic hybrid metal halides.
有机-无机杂化的锡（IV）基金属卤化物因其优异的结构稳定性而受到广泛关注。然而，实现具有高稳定性和高效光致发光（PL）效率的发红光的锡（IV）基金属卤化物仍然具有挑战性。在此，已获得一种具有零维（0D）结构的稳定的有机-无机锡（IV）基金属卤化物（CHON）SnCl，然而，由于Sn-4d电子的惰性表现和固有的间接带隙特征，其PL性能较差。为了应对上述挑战，将具有活性5s孤对电子的碲嵌入到（CHON）SnCl的晶格中，结果，具有直接带隙的5%Te掺杂的（CHON）SnCl表现出宽带深红色发射（688 nm），PL效率较高（53%）。实验和计算结果表明，碲的嵌入可以有效地调节（CHON）SnCl的能带结构，促进从间接带结构向直接带结构的转变，从而导致高效的辐射复合。受益于上述优点，使用Te掺杂的（CHON）SnCl制备了一种高效白光发光二极管（WLED），其超高显色指数（CRI）高达94.5，表明这种材料在固态照明方面具有巨大潜力。这项工作为有机-无机杂化金属卤化物高效发红光磷光体的设计提供了重要见解。
