Enhancing FRET through DNA-controlled Emitters and ENZ Metamaterials

Abstract

The ability to significantly enhance energy transfer processes at the nanoscale requires the simultaneous optimization of molecular-scale orientation and macroscopic photonic enhancement between multiple quantum emitters. However, achieving this dual control has remained a significant experimental challenge, often limited by the stochastic arrangement of emitter assemblies and spatially non-uniform electromagnetic fields in conventional photonic platforms. In this work, we demonstrate a unified architecture that achieves this synergy by combining the structural precision of DNA nanotechnology with the unique field environment generated by epsilon-near-zero (ENZ) materials. Using DNA molecular beacons as programmable emitter scaffolds, we establish fixed donor-acceptor separations and emitter orientations (Atto425/Cy3.5) in two well-defined conformational states: closed hairpin (emitter separation 2 nm) and extended (8.16 nm) configurations. These structures are then embedded in the near-field of a multilayer ENZ metamaterial substrate, which facilitates spatially uniform, enhanced electromagnetic field coupling. Time-resolved photoluminescence measurements demonstrate a significant increase in FRET efficiency for DNA-programmed emitter pairs in the ENZ environment, compared to those on a glass substrate, corresponding to increased donor quenching and shortened donor lifetime. These results establish a scalable experimental pathway for engineering light-matter interactions at molecular scales with applications in next-generation biosensing and quantum photonic technologies.