2. Academic Validation
  3. Single-molecule photoreaction quantitation through intraparticle-surface energy transfer (i-SET) spectroscopy

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

  • Nat Commun. 2020 Aug 27;11(1):4297. doi: 10.1038/s41467-020-18223-z.
Jian Zhou 1,  Changyu Li 1,  Denghao Li 1,  Xiaofeng Liu 1,  Zhao Mu 2,  Weibo Gao 2,  Jianrong Qiu 3,  Renren Deng 4 5
Affiliations

Affiliations

  • 1 Institute for Composites Science Innovation, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China.
  • 2 Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore, 637371, Singapore.
  • 3 State Key Laboratory of Modern Optical Instrumentation, College of Optical Science and Engineering, Zhejiang University, Hangzhou, 310027, China.
  • 4 Institute for Composites Science Innovation, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China. rdeng@zju.edu.cn.
  • 5 Key Laboratory for Organic Electronics and Information Displays, Institute of Advanced Materials, Nanjing University of Posts & Telecommunications, Nanjing, 210023, China. rdeng@zju.edu.cn.
PMID: 32855425 DOI: 10.1038/s41467-020-18223-z
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.

Figures
Products