Journal
NATURE COMMUNICATIONS
Volume 11, Issue 1, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-020-18223-z
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Funding
- National Key Research and Development Program of China [2018YFB0703803]
- Zhejiang Provincial National Natural Science Foundation of China [LR19B010002]
- National Natural Science Foundation of China [21801222, 51872256]
- Key Laboratory for Organic Electronics and Information Displays
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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. 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.
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