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

引用本文: 程子涵, 蒋凯, 蒋军, 王恒刚, 林恒伟. 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[J]. 物理化学学报, 2026, 42(2): 100169. doi: 10.1016/j.actphy.2025.100169 shu

Citation: Zihan Cheng, Kai Jiang, Jun Jiang, Henggang Wang, Hengwei Lin. Achieving thermal-stimulus-responsive dynamic afterglow from carbon dots by singlet-triplet energy gap engineering through covalent fixation[J]. Acta Physico-Chimica Sinica, 2026, 42(2): 100169. doi: 10.1016/j.actphy.2025.100169 shu

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.
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

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)

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(ΔE_ST)，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ΔE_ST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:

English

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

Zihan Cheng ^1, ,
Kai Jiang ^{1,
,} ,
Jun Jiang ^1, ,
Henggang Wang ^{1, 2,
,} ,
Hengwei Lin ^{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

Corresponding author: Email: jiangkai@jiangnan.edu.cn (Kai Jiang); wanghenggang11@163.com (Henggang Wang); linhengwei@jiangnan.edu.cn. Tel.: +86-510-8591-0225 (Hengwei Lin)

Received Date: 20 June 2025
Accepted Date: 19 August 2025
Revised Date: 11 August 2025
Available Online: 15 February 2026

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 (ΔE_ST) 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 ΔE_ST of CDs from 0.46 to 0.28 eV, as designed. This ΔE_ST 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:

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通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

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

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)

English

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

Corresponding author: Email: jiangkai@jiangnan.edu.cn (Kai Jiang); wanghenggang11@163.com (Henggang Wang); linhengwei@jiangnan.edu.cn. Tel.: +86-510-8591-0225 (Hengwei Lin)

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

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

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)

English

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

Corresponding author: Email: jiangkai@jiangnan.edu.cn (Kai Jiang); wanghenggang11@163.com (Henggang Wang); linhengwei@jiangnan.edu.cn. Tel.: +86-510-8591-0225 (Hengwei Lin)

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

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