Supramolecular Strategy for Constructing Mixed Coordination Units toward Ultra-Stable White-Light Emission in Zero-Dimensional Hybrid Indium Chloride

IF 8.7 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY ACS Materials Letters Pub Date : 2024-10-30 DOI:10.1021/acsmaterialslett.4c01744
Pei Wang, Qiqiong Ren, Nan Zhang, Guojun Zhou*, Shi-Li Li and Xian-Ming Zhang*, 
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Abstract

Intensive research into single-component white-light-emitting materials is extremely valuable for innovating next-generation solid-state lighting technology. Herein, we innovatively propose a crown ether-assisted supramolecular self-assembly strategy that is supported by the construction of mixed coordination units in low-dimensional hybrid metal halides (LHMHs). The resultant [(C10H20O5)InCl2]InCl4 is an extremely rare class of zero-dimensional (0D) indium-based chloride that is featured by the structurally deformable mixed coordination units of 7-coordinated [InCl2O5] (In-1) and 4-coordinated [InCl4] (In-2). Excitingly, it exhibits a high-quality white-light emission with a full width at half-maximum (fwhm) of 211 nm and a photoluminescence quantum yield (PLQY) of 33.6%, which is attributed to the unprecedented intrinsic dual self-trapped excitons (STEs) under electron–phonon coupling. The electron-transition mechanism is elucidated according to temperature-dependent PL spectra and theoretical calculations. Beyond that, the indium-based white-light emitter possesses superb water stability because of the hydrophobicity of 15-crown-5, which is unachievable for almost all LHMHs. This work sheds light on an executable self-assembly strategy for building mixed coordination units and extends to the design of single-component white-light-emitting materials.

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构建零维杂化氯化铟超稳定白光发射混合配位单元的超分子策略
深入研究单组分白光发光材料对于创新下一代固态照明技术是非常有价值的。在此,我们创新地提出了一种冠醚辅助的超分子自组装策略,该策略由低维杂化金属卤化物(LHMHs)中混合配位单元的构建支持。合成的[(C10H20O5)InCl2]InCl4是一类极为罕见的零维(0D)铟基氯化物,其特点是具有7-配位[InCl2O5] (In-1)和4-配位[InCl4] (In-2)的结构可变形混合配位单元。令人兴奋的是,它显示出高质量的白光发射,半峰全宽度(fwhm)为211 nm,光致发光量子产率(PLQY)为33.6%,这归因于前所未有的电子-声子耦合下的固有双自困激子(STEs)。根据温度相关的PL光谱和理论计算阐明了电子跃迁机理。除此之外,铟基白光发射器由于15-冠-5的疏水性而具有极好的水稳定性,这是几乎所有的LHMHs都无法实现的。这项工作揭示了一种可执行的自组装策略,用于构建混合协调单元,并扩展到单组分白光发光材料的设计。
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来源期刊
ACS Materials Letters
ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
14.60
自引率
3.50%
发文量
261
期刊介绍: ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.
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