Assembling programmable FRET-based photonic networks using designer DNA scaffolds

作者:Buckhout White Susan; Spillmann Christopher M; Algar W Russ; Khachatrian Ani; Melinger Joseph S; Goldman Ellen R; Ancona Mario G; Medintz Igor L*
来源:Nature Communications, 2014, 5(1): 5615.
DOI:10.1038/ncomms6615

摘要

DNA demonstrates a remarkable capacity for creating designer nanostructures and devices. A growing number of these structures utilize Forster resonance energy transfer (FRET) as part of the device%26apos;s functionality, readout or characterization, and, as device sophistication increases so do the concomitant FRET requirements. Here we create multi-dye FRET cascades and assess how well DNA can marshal organic dyes into nanoantennae that focus excitonic energy. We evaluate 36 increasingly complex designs including linear, bifurcated, Holliday junction, 8-arm star and dendrimers involving up to five different dyes engaging in four-consecutive FRET steps, while systematically varying fluorophore spacing by Forster distance (R-0). Decreasing R-0 while augmenting cross-sectional collection area with multiple donors significantly increases terminal exciton delivery efficiency within dendrimers compared with the first linear constructs. Forster modelling confirms that best results are obtained when there are multiple interacting FRET pathways rather than independent channels by which excitons travel from initial donor(s) to final acceptor.

  • 出版日期2014-12