Programmable Switching of Molecular Transitions via Plasmonic Toroidal Nanoantennae

Abstract

The ability to switch and program molecular transitions via deterministically located plasmonic nanoantennae presents opportunities for wide spectrum of applications from biosensors to quantum computing. Due to its topology, toroidal nanoantenna (TNA) focuses immense amount of three-dimensional (3D) local electric field by toroidal moment while allowing pre and post positioning around quantum emitters (QEs). Here, we report complete switching of molecular transition energies of quantum objects (QOs) with modulation depth of 99.9% over 2840-fold radiative enhancement. At optimized TNA geometries, Fano interference between the broadband plasmonic continuum and narrow quantum transitions of QOs suppresses both radiative and non-radiative decay channels near 850 nm, yielding an observable full switching that traps energy within the hybrid mode instead of re-emitting it. To show the promises of the concept, we further demonstrate systems with multiple QOs where spectral degeneracy enhances the transparency bandwidth, while detuning generates distinct minima, enabling individually addressable spectral responses. These results establish plasmonic TNA as a promising architecture for spectral detection of single or multi-molecule configurations with high sensitivity and empowers the user for the implementation of quantum mode switches to be used in photonic processing.