首页|期刊导航|物理化学学报|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OA

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

中文摘要英文摘要

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.

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.

程子涵;蒋凯;蒋军;王恒刚;林恒伟

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||河北师范大学化学与材料科学学院,河北 石家庄 050024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

化学化工

碳点热致变色余辉动态余辉刺激响应余辉共价固定

Carbon dotsThermochromic afterglowDynamic afterglowStimuli-responsive afterglowCovalent fixation

《物理化学学报》 2026 (2)

122-132,11

国家自然科学基金(52372047)资助项目

10.1016/j.actphy.2025.100169

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