Enhancement of single upconversion nanoparticle imaging by topologically segregated core-shell structure with inward energy migration.
Enhancement of single upconversion nanoparticle imaging by topologically segregated core-shell structure with inward energy migration.
复制标题
DOI：
10.1038/s41467-022-33660-8
复制
发表时间：
2022-10-07
影响因子：
16.6
通讯作者：
中科院分区：
文献类型：
--
作者：
操纵拓扑排列是调节天然光合作用蛋白质和人工聚合物中能量迁移的有力工具。在这里，我们报道了一种由NaErF4和NaYbF4组成的无机光学纳米系统，其中拓扑排列增强了上转换发光。考虑到纳米粒子内的能量迁移和能量转移，设计了三种体系结构：自外向内、由内向外和局部能量转移。从外到内的结构产生了最大的上转换发光，大约是单粒子水平上由内向外的6倍。蒙特卡罗模拟表明，拓扑相关的能量迁移有利于由外向内结构的上转换发光。与传统的核壳结构相比，优化的自外向内结构在单粒子水平上显示出上转换亮度提高了一个数量级以上，并用于活细胞中的长期单粒子跟踪。我们的发现使得合理的纳米探针工程能够用于单分子成像，并揭示了上转换纳米颗粒结构和光学性质之间的反直觉关系。操纵拓扑排列是调节分子体系和无机材料中能量迁移的有力工具。在这里，作者合成了不同结构的NaErF4和NaYbF4上转换纳米粒子，并展示了上转换发光的拓扑相关增强，与传统的核壳结构相比，亮度增加了一个数量级。
Manipulating topological arrangement is a powerful tool for tuning energy migration in natural photosynthetic proteins and artificial polymers. Here, we report an inorganic optical nanosystem composed of NaErF4 and NaYbF4, in which topological arrangement enhanced upconversion luminescence. Three architectures are designed for considerations pertaining to energy migration and energy transfer within nanoparticles: outside-in, inside-out, and local energy transfer. The outside-in architecture produces the maximum upconversion luminescence, around 6-times brighter than that of the inside-out at the single-particle level. Monte Carlo simulation suggests a topology-dependent energy migration favoring the upconversion luminescence of outside-in structure. The optimized outside-in structure shows more than an order of magnitude enhancement of upconversion brightness compared to the conventional core-shell structure at the single-particle level and is used for long-term single-particle tracking in living cells. Our findings enable rational nanoprobe engineering for single-molecule imaging and also reveal counter-intuitive relationships between upconversion nanoparticle structure and optical properties. Manipulating topological arrangement is a powerful tool for tuning the energy migration in molecular systems and inorganic materials. Here, authors synthesize NaErF4 and NaYbF4 upconversion nanoparticles with different architectures and demonstrate topology-dependent enhancement of upconversion luminescence, with up to an order of magnitude increase in brightness compared to conventional core-shell architectures.
登录
查看更多内容
上转换纳米颗粒：设计、纳米化学及其在治疗诊断学中的应用
影响因子：
62.1
作者：
Chen, Guanying;Qju, Hailong;Prasad, Paras N.;Chen, Xiaoyuan
通讯作者：
Chen, Xiaoyuan
影响因子：
4.9
作者：
Deria, Pravas;Yu, Jierui;White, Sandra N.
通讯作者：
White, Sandra N.
具有强上转换发光的均匀 NaLuF4 纳米粒子，用于植物细胞的无背景成像和痕量有机染料的超低功率检测
影响因子：
5.4
作者：
Hu, Shigang;Wu, Xiaofeng;Liu, Yunxin
通讯作者：
Liu, Yunxin
影响因子：
3.4
作者：
KUSUMI, A;SAKO, Y;YAMAMOTO, M
通讯作者：
YAMAMOTO, M
影响因子：
16.6
作者：
Gu, Yan;Sun, Wei;Fang, Ning
通讯作者：
Fang, Ning