Enabling Förster Resonance Energy Transfer from Large Nanocrystals through Energy Migration

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• 作者：Renren Deng ; Juan Wang ; Runfeng Chen ; Wei Huang ; Xiaogang Liu
• 刊名：Journal of the American Chemical Society
• 出版年：2016
• 出版时间：December 14, 2016
• 年：2016
• 卷：138
• 期：49
• 页码：15972-15979
• 全文大小：518K
• ISSN：1520-5126

文摘

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.