Efficient Circularly Polarized Luminescence from Mn–Br Hybrid Perovskite Assembled by Achiral Architectures

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2025-03-19 DOI:10.1002/anie.202425543
Lu Zhai, Jiayi Yuan, Jianyi Huang, Xue-Wei Pan, Li Wan, Weihua Ning, Xiao-Ming Ren
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Abstract

Circularly polarized luminescence (CPL)-active materials have attracted considerable attention due to their potential applications in various advanced technological fields. CPL activity typically requires compounds that crystallize in noncentrosymmetric chiral space groups. Achieving noncentrosymmetric crystal structures using achiral molecular architectures is highly appealing but remains a significant challenge. Herein, we present a strategy for designing and synthesizing high-performance CPL materials via crystallization-driven self-assembly using achiral architectures. We successfully obtained Mn2+-based halide enantiomeric hybrids (P-1 and M-1), self-assembled from [MnBr4]2− anions and rotational symmetric [Pr-dabco]2+ cations (Pr-dabco2+ = 1-propyl-1,4-diazabicyclo-[2.2.2]octan-1-ium), crystallizing in the chiral space group P212121. The single crystals of 1 exhibit exceptionally high CPL performance, with a luminescence dissymmetry factor |glum| and photoluminescence quantum yield (PLQY) up to 4.8 × 10−2 and 86.8%, respectively, thus a record-high figure of merit (FM) of 4.2 × 10−2 among reported Mn2+-based CPL materials. Furthermore, P/M-1 based UV-LED devices demonstrated outstanding light-emitting performance, including high color-purity, excellent stability, remarkable luminous brightness (74 591.94 cd m−2), and a high electroluminescence dissymmetry factor (glum) value of 3.2 × 10−2. This study offers a robust strategy for the design and development of high-performance CPL materials utilizing achiral molecular architectures.

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非手性结构组装Mn-Br杂化钙钛矿的高效圆极化发光
圆偏振发光活性材料因其在各种先进技术领域的潜在应用而受到广泛关注。CPL活性通常要求化合物在非中心对称的手性空间群中结晶。利用非手性分子结构实现非中心对称晶体结构是非常有吸引力的,但仍然是一个重大的挑战。在此,我们提出了一种利用非手性结构通过结晶驱动自组装设计和合成高性能CPL材料的策略。我们成功地获得了由[MnBr4]2-阴离子和旋转对称的[Pr-dabco]2+阳离子(Pr-dabco + = 1-丙基-1,4-重氮杂环-[2.2.2]辛烷-1-ium)自组装的Mn2+基卤化物对映体杂化体(P-1和M-1),并在P212121的手性空间群中结晶。1的单晶表现出非常高的CPL性能,发光不对称因子|glum|和光致发光量子产率(PLQY)分别高达4.8×10-2和86.8%,因此在报道的Mn2+基CPL材料中,品质指数(FM) 4.2×10-2创历史新高。此外,基于P/M-1的UV-LED器件具有出色的发光性能,包括高色纯度,优异的稳定性,显着的发光亮度(74,591.94 cd m-2)和高电致发光不对称因子(glum)值3.6×10-2。本研究为利用非手性分子结构设计和开发高性能CPL材料提供了强有力的策略。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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