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通过整合n-π*/π-π*跃迁,亮态三重态激子可实现有机小分子的高性能白光发射。

Brightening triplet excitons enable high-performance white-light emission in organic small molecules via integrating n-π*/π-π* transitions.

作者信息

Yang Qing, Yang Xinyi, Wang Yixuan, Fei Yunfan, Li Fang, Zheng Haiyan, Li Kuo, Han Yibo, Hattori Takanori, Zhu Pinwen, Zhao Shuaiqiang, Fang Leiming, Hou Xuyuan, Liu Zhaodong, Yang Bing, Zou Bo

机构信息

State Key Laboratory of Superhard Materials, Synergetic Extreme Condition High-Pressure Science Center, College of Physics, Jilin University, Changchun, China.

Center for High Pressure Science and Technology Advanced Research, Beijing, China.

出版信息

Nat Commun. 2024 Sep 5;15(1):7778. doi: 10.1038/s41467-024-52196-7.

Abstract

Luminescent materials that simultaneously embody bright singlet and triplet excitons hold great potential in optoelectronics, signage, and information encryption. However, achieving high-performance white-light emission is severely hampered by their inherent unbalanced contribution of fluorescence and phosphorescence. Herein, we address this challenge by pressure treatment engineering via the hydrogen bonding cooperativity effect to realize the mixture of n-π*/π-π* transitions, where the triplet state emission was boosted from 7% to 40% in isophthalic acid (IPA). A superior white-light emission based on hybrid fluorescence and phosphorescence was harvested in pressure-treated IPA, and the photoluminescence quantum yield was increased to 75% from the initial 19% (blue-light emission). In-situ high-pressure IR spectra, X-ray diffraction, and neutron diffraction reveal continuous strengthening of the hydrogen bonds with the increase of pressure. Furthermore, this enhanced hydrogen bond is retained down to the ambient conditions after pressure treatment, awarding the targeted IPA efficient intersystem crossing for balanced singlet/triplet excitons population and resulting in efficient white-light emission. This work not only proposes a route for brightening triplet states in organic small molecules, but also regulates the ratio of singlet and triplet excitons to construct high-performance white-light emission.

摘要

同时体现明亮单重态和三重态激子的发光材料在光电子学、标识和信息加密方面具有巨大潜力。然而,其固有的荧光和磷光贡献不平衡严重阻碍了高性能白光发射的实现。在此,我们通过基于氢键协同效应的压力处理工程来应对这一挑战,以实现n-π*/π-π*跃迁的混合,其中间苯二甲酸(IPA)中的三重态发射从7%提高到了40%。在经过压力处理的IPA中获得了基于混合荧光和磷光的优异白光发射,光致发光量子产率从初始的19%(蓝光发射)提高到了75%。原位高压红外光谱、X射线衍射和中子衍射表明,随着压力的增加,氢键不断增强。此外,这种增强的氢键在压力处理后一直保持到环境条件,赋予目标IPA有效的系间窜越,以平衡单重态/三重态激子数量并产生高效的白光发射。这项工作不仅提出了一种在有机小分子中增强三重态的途径,还调节了单重态和三重态激子的比例以构建高性能白光发射。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4d47/11377787/d6dda7d39d94/41467_2024_52196_Fig1_HTML.jpg

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