Collective Blinking of Upconversion Emission in Lanthanide-doped Nanocrystals
Abstract
Fluorescence blinking, often regarded as a limitation for stable emitters, can enable super-resolution localization microscopy and serve as a versatile reporter of the photophysical states of quantum emitters and their interactions with local environment. However, conventional blinking emitters are typically single quantum systems with Stokes-shifted fluorescence, making them susceptible to autofluorescence background, weak signal, and irreversible photodegradation under prolonged excitation. In contrast, single lanthanide-doped upconversion nanocrystals are effectively background-free anti-Stokes emitters and demonstrate robust resistance to photodegradation, yet they are generally considered non-blinking owing to the presence of a large ensemble of uncorrelated emitting lanthanide ions within a single nanocrystal. Here we report the discovery and control of collective blinking in the upconversion luminescence of thousands of lanthanide ions within a single nanocrystal. The blinking exhibits on-off intensity ratio exceeding 10, persists for over 15 hours (over 10,000 cycles) without discernible photodegradation, and can be reversibly controlled by adjusting the excitation power. We elucidate a universal, activator-independent upconversion blinking mechanism, whereby a single quencher, stochastically generated via a cooperative multi-ion process, can intercept delocalized excitation energy within the Yb3+ sensitizer network and darken the whole nanocrystal. Benefiting from the high-contrast, long-term photostable blinking and background-free emission, we achieve robust super-resolution localization microscopy that resolves individual nanocrystals in aggregates with 1.2 nm precision. This work establishes a general strategy to realize and control collective blinking in photostable multi-emitter nanosystems, opening new opportunities in nanoscience, bioimaging, and quantum technologies.
Versions
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BibTeX
@misc{ma2026collective,
title = {{Collective Blinking of Upconversion Emission in Lanthanide-doped Nanocrystals}},
author = {Tianzi Ma and Dingxin Huang and Yongjun Meng and Jianwei Tang and Feng Li and Yihao Yu and Xiaorong Zhang and Guanying Chen and Xue-Wen Chen},
howpublished = {arXiv},
year = {2026},
month = aug,
doi = {10.48550/arxiv.2608.16244},
eprint = {2608.16244},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2608.16244},
}
RIS
TY - UNPB
TI - Collective Blinking of Upconversion Emission in Lanthanide-doped Nanocrystals
AU - Tianzi Ma
AU - Dingxin Huang
AU - Yongjun Meng
AU - Jianwei Tang
AU - Feng Li
AU - Yihao Yu
AU - Xiaorong Zhang
AU - Guanying Chen
AU - Xue-Wen Chen
PY - 2026
DA - 2026/08/17
PB - arXiv
DO - 10.48550/arxiv.2608.16244
UR - https://arxiv.org/abs/2608.16244
AB - Fluorescence blinking, often regarded as a limitation for stable emitters, can enable super-resolution localization microscopy and serve as a versatile reporter of the photophysical states of quantum emitters and their interactions with local environment. However, conventional blinking emitters are typically single quantum systems with Stokes-shifted fluorescence, making them susceptible to autofluorescence background, weak signal, and irreversible photodegradation under prolonged excitation. In contrast, single lanthanide-doped upconversion nanocrystals are effectively background-free anti-Stokes emitters and demonstrate robust resistance to photodegradation, yet they are generally considered non-blinking owing to the presence of a large ensemble of uncorrelated emitting lanthanide ions within a single nanocrystal. Here we report the discovery and control of collective blinking in the upconversion luminescence of thousands of lanthanide ions within a single nanocrystal. The blinking exhibits on-off intensity ratio exceeding 10, persists for over 15 hours (over 10,000 cycles) without discernible photodegradation, and can be reversibly controlled by adjusting the excitation power. We elucidate a universal, activator-independent upconversion blinking mechanism, whereby a single quencher, stochastically generated via a cooperative multi-ion process, can intercept delocalized excitation energy within the Yb3+ sensitizer network and darken the whole nanocrystal. Benefiting from the high-contrast, long-term photostable blinking and background-free emission, we achieve robust super-resolution localization microscopy that resolves individual nanocrystals in aggregates with 1.2 nm precision. This work establishes a general strategy to realize and control collective blinking in photostable multi-emitter nanosystems, opening new opportunities in nanoscience, bioimaging, and quantum technologies.
ER -