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【唐本忠先生七秩华诞专辑】酸碱和客体可调控的延迟荧光及其逻辑门应用

宋奎柱1,龙宇杰1,2,王亚茹1,王嘉麒1,2,吕海燕1,陈传峰1,2   

  1. 1. 中国科学院大学 2. 中国科学院化学研究所分子识别与功能重点实验室,北京分子科学国家实验室

  • 收稿日期:2025-12-16 修回日期:2026-02-24 出版日期:2026-03-10 发布日期:2026-03-10
  • 通讯作者: 陈传峰 E-mail:cchen@iccas.ac.cn
  • 基金资助:
    国家自然科学基金(批准号:22371277, 22031010, 22171272)和中国科学院战略性前沿专项(批准号:XDB0520302)资助

Acid/Base and Guest Controlled Delayed Fluorescence and Its Application in Logic Gate

SONG Kuizhu1,LONG Yujie1,2,WANG Yaru1,WANG Jiaqi1,2,LU Haiyan1,CHEN Chuanfeng1,2   

  1. 1. University of Chinese Academy of Sciences 2. Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Molecular Recognition and Function, Institute of Chemistry, Chinese Academy of Sciences

  • Received:2025-12-16 Revised:2026-02-24 Online:2026-03-10 Published:2026-03-10
  • Contact: Chuan-Feng Chen E-mail:cchen@iccas.ac.cn
  • Supported by:
    Supported by the National Natural Science Foundation of China (Nos.22371277, 22031010, 22171272) and the Strategic Priority Research Program of the Chinese Academy of Sciences, China (No.XDB0520302)

摘要: 报道了一种通过主-客体作用与酸碱刺激调控空间电荷转移(TSCT)路径的延迟荧光体系. 在大环分子C[3]A-1中,空腔内3-氰基吡啶受体与大环给体之间形成分子内TSCT通道,产生绿色热激活延迟荧光(TADF)发射. 引入客体2-氰基吡嗪(2-CP)后,主-客体组装诱导受体构象变化,使分子内TSCT路径关闭,并在客体与大环侧壁之间构建新的分子间TSCT通道,体系呈现黄色TADF发射,实现延迟荧光的可逆切换. 此外,受体氮位点的质子化/去质子化赋予体系酸碱响应性,可实现发光的可逆开关. 基于多重刺激响应特性,成功构建了多级分子逻辑门,为可调控延迟荧光材料的设计提供了新思路.

关键词: 主客体作用, 空间电荷转移, 刺激响应性, 热激活延迟荧光, 杯[3]二氢吖啶

Abstract: A delayed fluorescence system regulating the space charge transfer (TSCT) pathway via host-guest interactions and acid-base stimulation is proposed. Within the macrocyclic molecule C[3]A-1,an intramolecular TSCT pathway forms between the 3-cyanopyridine acceptor in the cavity and the macrocyclic donor,generating green thermally activated delayed fluorescence (TADF) emission. Upon introduction of the guest 2-cyanopyrazine (2-CP),host-guest assembly induces a conformational change in the receptor,shutting down the intramolecular TSCT pathway. Simultaneously,a new intermolecular TSCT pathway is established between the guest and the macrocycle sidewall, leading to yellow TADF emission and enabling reversible switching of delayed fluorescence,Furthermore,protonation/deprotonation at the receptor's nitrogen site confers acid-base responsiveness,enabling reversible switching of luminescence. Leveraging these multi-stimulus-responsive properties,a multi-level molecular logic gate was successfully constructed, offering novel insights for designing tunable delayed-fluorescence materials.

Key words: Host-guest interaction, TSCT, Stimulus response, TADF, Calix[3]acridans

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