State Key Laboratory of Luminescence and Applications, Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, Changchun, 130033, China.
University of the Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2018 Mar 12;57(12):3054-3058. doi: 10.1002/anie.201711606. Epub 2018 Feb 14.
Upconversion emission dynamics have long been believed to be determined by the activator and its interaction with neighboring sensitizers. Herein this assumption is, however, shown to be invalid for nanostructures. We demonstrate that excitation energy migration greatly affects upconversion emission dynamics. "Dopant ions' spatial separation" nanostructures are designed as model systems and the intimate link between the random nature of energy migration and upconversion emission time behavior is unraveled by theoretical modelling and confirmed spectroscopically. Based on this new fundamental insight, we have successfully realized fine control of upconversion emission time behavior (either rise or decay process) by tuning the energy migration paths in various specifically designed nanostructures. This result is significant for applications of this type of materials in super resolution spectroscopy, high-density data storage, anti-counterfeiting, and biological imaging.
上转换发射动力学长期以来一直被认为取决于激活剂及其与邻近敏化剂的相互作用。然而，在此假设对于纳米结构是无效的。我们证明了激发能量迁移极大地影响了上转换发射动力学。“掺杂离子的空间分离”纳米结构被设计为模型体系，通过理论建模和光谱学证实，揭示了能量迁移的随机性质与上转换发射时间行为之间的紧密联系。基于这一新的基本见解，我们通过调整各种特定设计的纳米结构中的能量迁移路径，成功地实现了对上转换发射时间行为（无论是上升还是衰减过程）的精细控制。这一结果对于这类材料在超分辨光谱学、高密度数据存储、防伪和生物成像中的应用具有重要意义。
