title: Enabling Förster Resonance Energy Transfer from Large Nanocrystals through Energy Migration.
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.
authors.affiliation: Department of Chemistry, National University of Singapore , Singapore 117543.
authors.forename: Renren
authors.initials: R
authors.lastname: Deng
authors.affiliation: Department of Chemistry, National University of Singapore , Singapore 117543.
authors.forename: Juan
authors.initials: J
authors.lastname: Wang
authors.affiliation: Key Laboratory for Organic Electronics and Information Displays & Institute of Advanced Materials, Jiangsu National Synergetic Innovation Center for Advanced Materials, Nanjing University of Posts and Telecommunications , Nanjing 210023, China.
authors.forename: Runfeng
authors.initials: R
authors.lastname: Chen
authors.affiliation: Key Laboratory for Organic Electronics and Information Displays & Institute of Advanced Materials, Jiangsu National Synergetic Innovation Center for Advanced Materials, Nanjing University of Posts and Telecommunications , Nanjing 210023, China.|Key Laboratory of Flexible Electronics and Institute of Advanced Materials, Jiangsu National Synergetic Innovation Center for Advanced Materials, Nanjing Tech University , Nanjing 211816, China.
authors.forename: Wei
authors.initials: W
authors.lastname: Huang
authors.affiliation: Department of Chemistry, National University of Singapore , Singapore 117543.|Institute of Materials Research and Engineering , Singapore 138634.
authors.forename: Xiaogang
authors.initials: X
authors.lastname: Liu