Single-molecule photoreaction quantitation through intraparticle-surface energy transfer (i-SET) spectroscopy

Quantification of nanoparticle-molecule interaction at a single-molecule level remains a daunting challenge, mainly due to ultra-weak emission from single molecules and the perturbation of the local environment. Here we report the rational design of an intraparticle-surface energy transfer (i-SET) p...

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Bibliographic Details
Published in:Nature communications 2020-08, Vol.11 (1), p.4297-4297, Article 4297
Main Authors: Zhou, Jian, Li, Changyu, Li, Denghao, Liu, Xiaofeng, Mu, Zhao, Gao, Weibo, Qiu, Jianrong, Deng, Renren
Format: Article
Language:English
Subjects:
639/624/1107/510
639/624/399/354
639/925/357/354
639/925/930/527/2047
9/10
Chemical compounds
Design
Detection
Energy transfer
Fluorescence
Fluorophores
Humanities and Social Sciences
multidisciplinary
Nanoparticles
Perturbation
Probes
Quantitation
Science
Science (multidisciplinary)
Spectral sensitivity
Spectroscopy
Spectrum analysis
Surface energy
Surface properties
Upconversion
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Summary:Quantification of nanoparticle-molecule interaction at a single-molecule level remains a daunting challenge, mainly due to ultra-weak emission from single molecules and the perturbation of the local environment. Here we report the rational design of an intraparticle-surface energy transfer (i-SET) process, analogous to high doping concentration-induced surface quenching effects, to realize single-molecule sensing by nanoparticle probes. This design, based on a Tb 3+ -activator-rich core-shell upconversion nanoparticle, enables a much-improved spectral response to fluorescent molecules at single-molecule levels through enhanced non-radiative energy transfer with a rate over an order of magnitude faster than conventional counterparts. We demonstrate a quantitative analysis of spectral changes of one to four fluorophores tethered on a single nanoparticle through i-SET spectroscopy. Our results provide opportunities to identify photoreaction kinetics at single-molecule levels and provide direct information for understanding behaviors of individual molecules with unprecedented sensitivity. Single-molecule sensing is very challenging due to weak emitted signals and environmental interference. Here the authors design a method (i-SET) for single molecule sensing with core-shell upconverting nanoparticles, which relies on signal enhancement by the activator-rich probes to quantify fluorophores attached to a single nanoparticle.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-020-18223-z