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Tunable Fluorescence from Dye‐Modified DNA‐Assembled Plasmonic Nanocube Arrays

Colloidal crystal engineering with DNA on template‐confined surfaces is used to prepare arrays of nanocube‐based plasmonic antennas and deliberately place dyes with sub‐nm precision into their hotspots, on the DNA bonds that confine the cubes to the underlying gold substrate. This combined top‐down and bottom‐up approach provides independent control over both the plasmonic gap and photonic lattice modes of the surface‐confined particle assemblies and allows for the tuning of the interactions between the excited dyes and plasmonically active antennas. Furthermore, the gap mode of the antennas can be modified in situ by utilizing the solvent‐dependent structure of the DNA bonds. This is studied by placing two dyes, with different emission wavelengths, under the nanocubes and recording their solvent‐dependent emission. It is shown that dye emission not only depends upon the in‐plane structure of the antennas but also the size of the gap, which is regulated with solvent. Importantly, this approach allows for the systematic understanding of the relationship between nanoscale architecture and plasmonically coupled dye emission, and points toward the use of colloidal crystal engineering with DNA to create stimuli responsive architectures, which can find use in chemical sensing and tunable light sources.