Open AccessUnderstanding Förster Resonance Energy Transfer in the Sheet Regime with DNA Brick-Based Dye Networks
Author(s) -
Divita Mathur,
Anirban Samanta,
Mario G. Ancona,
Sebastián A. Dı́az,
Young-Chan Kim,
Joseph S. Melinger,
Ellen R. Goldman,
John Sadowski,
Luvena L. Ong,
Peng Yin,
Igor L. Medintz
Publication year - 2021
Publication title -
acs nano
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.554
H-Index - 382
eISSN - 1936-086X
pISSN - 1936-0851
DOI - 10.1021/acsnano.1c05871
Subject(s) - förster resonance energy transfer , acceptor , materials science , resonance (particle physics) , nanotechnology , energy transfer , energy (signal processing) , chemical physics , block (permutation group theory) , biological system , fluorescence , physics , optics , atomic physics , quantum mechanics , condensed matter physics , geometry , mathematics , biology
Controlling excitonic energy transfer at the molecular level is a key requirement for transitioning nanophotonics research to viable devices with the main inspiration coming from biological light-harvesting antennas that collect and direct light energy with near-unity efficiency using Förster resonance energy transfer (FRET). Among putative FRET processes, point-to-plane FRET between donors and acceptors arrayed in two-dimensional sheets is predicted to be particularly efficient with a theoretical 1/ r 4 energy transfer distance ( r ) dependency versus the 1/ r 6 dependency seen for a single donor-acceptor interaction. However, quantitative validation has been confounded by a lack of robust experimental approaches that can rigidly place dyes in the required nanoscale arrangements. To create such assemblies, we utilize a DNA brick scaffold, referred to as a DNA block, which incorporates up to five two-dimensional planes with each displaying from 1 to 12 copies of five different donor, acceptor, or intermediary relay dyes. Nanostructure characterization along with steady-state and time-resolved spectroscopic data were combined with molecular dynamics modeling and detailed numerical simulations to compare the energy transfer efficiencies observed in the experimental DNA block assemblies to theoretical expectations. Overall, we demonstrate clear signatures of sheet regime FRET, and from this we provide a better understanding of what is needed to realize the benefits of such energy transfer in artificial dye networks along with FRET-based sensing and imaging.