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

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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
    Nanjing University of Posts & Telecommunications)

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.

Suggested Citation

  • Jian Zhou & Changyu Li & Denghao Li & Xiaofeng Liu & Zhao Mu & Weibo Gao & Jianrong Qiu & Renren Deng, 2020. "Single-molecule photoreaction quantitation through intraparticle-surface energy transfer (i-SET) spectroscopy," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-18223-z
    DOI: 10.1038/s41467-020-18223-z
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