Enhancement of single upconversion nanoparticle imaging by topologically segregated core-shell structure with inward energy migration

Yanxin Zhang, Rongrong Wen, Jialing Hu, Daoming Guan, Xiaochen Qiu, Yunxiang Zhang (), Daniel S. Kohane () and Qian Liu ()
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Yanxin Zhang: Fudan University
Rongrong Wen: Fudan University
Jialing Hu: Fudan University
Daoming Guan: Fudan University
Xiaochen Qiu: Fudan University
Yunxiang Zhang: Fudan University
Daniel S. Kohane: Harvard Medical School
Qian Liu: Fudan University

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: Abstract 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.

Date: 2022
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DOI: 10.1038/s41467-022-33660-8

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