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Enabling Förster Resonance Energy Transfer from Large Nanocrystals through Energy Migration

Author:
Deng, Renren, Wang, Juan, Chen, Runfeng, Huang, Wei, Liu, Xiaogang
Source:
Journal of the American Chemical Society 2016 v.138 no.49 pp. 15972-15979
ISSN:
1520-5126
Subject:
energy transfer, image analysis, models, nanocrystals, particle size
Abstract:
The stringent distance dependence of Förster resonance energy transfer (FRET) has limited the ability of an energy donor to donate excitation energy to an acceptor over a Förster critical distance (R₀) of 2–6 nm. This poses a fundamental size constraint (<8 nm or ∼4R₀) for experimentation requiring particle-based energy donors. Here, we describe a spatial distribution function model and theoretically validate that the particle size constraint can be mitigated through coupling FRET with a resonant energy migration process. By combining excitation energy migration and surface trapping, we demonstrate experimentally an over 600-fold enhancement over acceptor emission for large nanocrystals (30 nm or ∼15R₀) with surface-anchored molecular acceptors. Our work shows that the migration-coupled approach can dramatically improve sensitivity in FRET-limited measurement, with potential applications ranging from facile photochemical synthesis to biological sensing and imaging at the single-molecule level.
Agid:
5594319