Gong Jiacheng, Zhou Wusen, Li Zhuo, Li Xingjun, Yuan Wen, Gu Xiaobo, Niu Qianqian, Liu Yan, Xu Jin, Li Renfu, Tu Datao, Lu Shan, Chen Xueyuan
State Key Laboratory of Structural Chemistry and Fujian Key Laboratory of Nanomaterials, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, China.
Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou, Fujian, 350108, China.
Adv Sci (Weinh). 2025 Jul;12(27):e2503110. doi: 10.1002/advs.202503110. Epub 2025 May 2.
Near-infrared (NIR) dyes can overcome the weak absorption of lanthanide nanoparticles (NPs) by antenna sensitization, offering new avenues to develop efficient and versatile lanthanide nanomaterials. However, current research on dye-sensitized lanthanide NPs for photothermal conversion is still preliminary, and the involved excited-state dynamics and interfacial interactions remain elusive. Herein, steady-state/transient absorption spectroscopy and theoretical calculation are used to investigate the coordination and aggregation states of cypate dyes on NaNdF NPs, revealing the influence of interfacial interactions on resonant energy transfer. Synergetic heat-generation mechanism of lanthanide cross-relaxation and dye intermolecular collisions is further proposed. The photothermal conversion efficiency of cypate-NaNdF nanocomposites reaches 50.4%, outperforming those of typical photothermal materials with high NIR absorption. Moreover, the intersystem crossing of cypate can be inhibited due to the depopulation of the S exciton via ET, thereby improving anti-photobleaching ability. These dye-sensitized NaNdF nanocomposites exhibit superior photothermal effect, stability and NIR-II luminescence, showing great potential in theranostic applications.
近红外（NIR）染料可通过天线敏化克服镧系纳米颗粒（NPs）吸收较弱的问题，为开发高效且通用的镧系纳米材料提供了新途径。然而，目前关于用于光热转换的染料敏化镧系NPs的研究仍处于初步阶段，其中涉及的激发态动力学和界面相互作用仍不明确。在此，利用稳态/瞬态吸收光谱和理论计算研究了cypate染料在NaNdF NPs上的配位和聚集状态，揭示了界面相互作用对共振能量转移的影响。进一步提出了镧系交叉弛豫和染料分子间碰撞的协同发热机制。cypate-NaNdF纳米复合材料的光热转换效率达到50.4%，优于具有高近红外吸收的典型光热材料。此外，由于通过电子转移使S激子去填充，cypate的系间窜越可受到抑制，从而提高抗光漂白能力。这些染料敏化的NaNdF纳米复合材料表现出优异的光热效应、稳定性和近红外二区发光，在诊疗应用中显示出巨大潜力。
