物理化学学报 >> 2026, Vol. 42 >> Issue (2): 100169.doi: 10.1016/j.actphy.2025.100169

所属专题： 碳点功能材料

论文 上一篇    下一篇

通过共价固定调控单重态-三重态能隙实现碳点热刺激响应动态余辉

程子涵1, 蒋凯1,*(), 蒋军1, 王恒刚1,2,*(), 林恒伟1,*()   

  1. 1 江南大学化学与材料工程学院, 光响应分子与材料国际联合研究中心, 江苏 无锡 214122
    2 河北师范大学化学与材料科学学院, 河北 石家庄 050024
  • 收稿日期:2025-06-20 修回日期:2025-08-11 录用日期:2025-08-19 发布日期:2025-12-03
  • 通讯作者: Email: jiangkai@jiangnan.edu.cn (蒋凯)wanghenggang11@163.com (王恒刚)linhengwei@jiangnan.edu.cn. Tel.: +86-510-8591-0225 (林恒伟)

Achieving thermal-stimulus-responsive dynamic afterglow from carbon dots by singlet-triplet energy gap engineering through covalent fixation

Zihan Cheng1, Kai Jiang1,*(), Jun Jiang1, Henggang Wang1,2,*(), Hengwei Lin1,*()   

  1. 1 International Joint Research Center for Photo-responsive Molecules and Materials, School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, Jiangsu Province, China
    2 Chemistry Postdoctoral Research Station at Hebei Normal University, College of Chemistry and Materials Science, Hebei Normal University, Shijiazhuang 050024, Hebei Province, China
  • Received:2025-06-20 Revised:2025-08-11 Accepted:2025-08-19 Published:2025-12-03
  • Contact: Email: jiangkai@jiangnan.edu.cn (Kai Jiang)wanghenggang11@163.com (Henggang Wang)linhengwei@jiangnan.edu.cn. Tel.: +86-510-8591-0225 (Hengwei Lin)

RichHTML

12

PDF

142

赞

补充材料

1

摘要：

刺激响应发光与动态发射特性的结合，可构建多级认证系统，为增强信息加密安全性提供新策略。通过合理调控材料的单线态-三线态能隙(ΔEST)，可同时激活磷光(Phos)与延迟荧光(DF)，实现可编程的动态余辉行为。本研究将碳点(CDs)原位共价固定在三聚氰酸基质中，率先报道了基于CDs的热响应动态余辉材料。该材料在宽温域(273.15–423.15 K)内呈现热驱动的绿色至蓝色余辉转变，同时具有热致变色余辉(TCA)与时间分辨余辉(TRA)双重模式的动态余辉特性。值得注意的是，该材料在348.15 K阈值温度以上发生蓝色至绿余辉逆转，此时热驱动的激子分布使TRA效应占据主导。这种TCA-TRA协同作用赋予材料前所未有的动态余辉调控能力。结构与光物理分析证实：原位共价固定按计划使CDs的ΔEST从0.46 eV降至0.28 eV。该能隙调控实现了对Phos/DF平衡的热调节，直接主导了所观测到的动态余辉性能。最后，本研究展示了该材料在热监测与高安全性信息保护领域的应用潜力。

关键词: 碳点, 热致变色余辉, 动态余辉, 刺激响应余辉, 共价固定

Abstract:

Integrating stimuli-responsive luminescence with dynamic emission properties offers a powerful strategy to enhance information encryption through multi-level authentication systems. By rationally tuning the singlet-triplet energy gap (ΔEST) of a material, simultaneous activation of phosphorescence (Phos) and delayed fluorescence (DF) can be achieved, enabling programmable dynamic afterglow behavior. In this work, we report the first carbon dot (CD)-based thermoresponsive dynamic afterglow material, synthesized via in situ covalent immobilization of CDs within a cyanuric acid matrix. The resulting system demonstrates a thermally driven green-to-blue afterglow transition across a wide temperature range (273.15–423.15 K), exhibiting dual-mode thermochromic afterglow (TCA) and time-resolved afterglow (TRA) characteristics. Notably, a blue-to-green afterglow transition occurs above the threshold temperature of 348.15 K, where TRA dominates due to temperature-dependent exciton redistribution. This synergistic TCA-TRA interplay endows the material with unprecedented dynamic afterglow modulation capabilities. Structural and photophysical analyses confirm that covalent fixation reduces the ΔEST of CDs from 0.46 to 0.28 eV, as designed. This ΔEST engineering enables thermal control over the Phos/DF equilibrium, directly governing the observed dynamic emission. Finally, the potential applications of the prepared material in thermal monitoring and high-security information protection are also demonstrated.

Key words: Carbon dots, Thermochromic afterglow, Dynamic afterglow, Stimuli-responsive afterglow, Covalent fixation