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Lone Pairs-Mediated Multiple Through-Space Interactions for Efficient Room-Temperature Phosphorescence

Fulong MaDepartment of Chemistry, Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong 999077, ChinaBo WuSiwei ZhangSchool of Science and Engineering, Shenzhen Institute of Aggregate Science and TechnologyJinhui JiangSchool of Science and Engineering, Shenzhen Institute of Aggregate Science and TechnologyJinghong ShiDepartment of Chemistry, Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong 999077, ChinaZeyang DingSchool of Science and Engineering, Shenzhen Institute of Aggregate Science and TechnologyYue ZhangSchool of Science and Engineering, Shenzhen Institute of Aggregate Science and TechnologyHaozhe TanSchool of Science and Engineering, Shenzhen Institute of Aggregate Science and TechnologyParvej AlamSchool of Science and Engineering, Shenzhen Institute of Aggregate Science and TechnologyJacky W. Y. LamDepartment of Chemistry, Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong 999077, ChinaYu XiongCenter for AIE Research, Shenzhen Key Laboratory of Polymer Science and Technology, Guangdong Research Center for Interfacial Engineering of Functional Materials, College of Materials Science and EngineeringZhen LiHubei Key Lab on Organic and Polymeric Optoelectronic Materials, Sauvage Center for Molecular Sciences, Department of ChemistryBen Zhong TangDepartment of Chemistry, Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong 999077, ChinaZheng ZhaoSchool of Science and Engineering, Shenzhen Institute of Aggregate Science and Technology
2025en
ABI

Аннотация

The simultaneous generation and stabilization of triplet excitons are the key to realizing efficient organic room temperature phosphorescence (RTP), which is challenging owing to the obscure mechanism and structure–property relationships. Herein, a strategy of lone-pair-mediated multiple through-space interactions (TSIs) is proposed to availably induce RTP. By incorporating heteroatoms to facilitate through-space n–n and n−π interactions, the lone pairs are delocalized throughout the structure, resulting in the dense splitting of the excited-state energy levels. Thus, more matched energy levels with a small energy gap between singlet and triplet states (ΔEST) emerge, resulting in multiple intersystem crossing (ISC) transition channels that assist triplet excitons generation. The strong TSIs also effectively rigidify the molecular structures and thus stabilize triplet excitons for radiation. Furthermore, the manipulation of TSI intensity allows efficiency enhancement, persistent time prolongation, and tolerance to high temperatures of RTP. This work not only explores the fundamental principle of the RTP mechanism from a new view but also provides a universal strategy for ISC promotion and triple excitons stabilization.

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