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Plasmonically enhanced fluorescence is a widely studied and appliedphenomenon, however only a comparative theoretical and experimental analyses ofcoupled fluorophores and plasmonic nanoresonators makes it possible to uncover,how this phenomenon can be controlled. A numerical optimization method wasapplied to design configurations that are capable of resulting in anenhancement of excitation and emission, moreover of both phenomenasimultaneously in coupled Cy5 dye molecule and gold nanorod systems. Parametricsensitivity studies revealed, how the fluorescence enhancement depends on themolecule's location, distance and orientation. Coupled systems designed forsimultaneous improvement exhibited the highest (intermediate directional) totalfluorescence enhancement, which is accompanied by intermediate sensitivity tothe molecule's parameters, except the location and orientation sensitivity atthe excitation wavelength. Gold nanorods with a geometry corresponding to thepredicted optimal configurations were synthesized, and DNA strands were used tocontrol the Cy5 dye molecule distance from the nanorod surface viahybridization of the Cy5-labelled oligonucleotide. State-of-the-art dSTORMmicroscopy was used to accomplish a proof-of-concept experimental demonstrationof the theoretically predicted (directional) total fluorescence enhancement.The measured fluorescence enhancement was in good agreement with theoreticalpredictions, thus providing a complete kit to design and prepare couplednanosystems exhibiting plasmonically enhanced fluorescence.

Mapping fluorescence enhancement of plasmonic nanorod coupled dye molecules