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

Jian Zhou, Changyu Li, Denghao Li, Xiaofeng Liu, Zhao Mu, Weibo Gao, Jianrong Qiu and Renren Deng ()
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Jian Zhou: Zhejiang University
Changyu Li: Zhejiang University
Denghao Li: Zhejiang University
Xiaofeng Liu: Zhejiang University
Zhao Mu: Nanyang Technological University
Weibo Gao: Nanyang Technological University
Jianrong Qiu: Zhejiang University
Renren Deng: Zhejiang University

Nature Communications, 2020, vol. 11, issue 1, 1-8

Abstract: Abstract 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 Tb3+-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.

Date: 2020
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DOI: 10.1038/s41467-020-18223-z

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