3D DNA origami-enabled molecularly addressable optical nanocircuit.

Clusters of nanoparticles enable electric and magnetic resonances and strong light-molecule interactions, including plasmonic resonance energy transfer (PRET). The optical nanocircuit concept provides a predictive RLC framework for these responses, but experimental realization has been limited by insufficient control over nanogaps and molecular placement. Here, we introduce a molecularly addressable optical nanocircuit based on a robust three-dimensional (3D) DNA origami. We demonstrate that gold nanoparticles and dye-loaded origami function as distinct circuit elements, with the latter acting as a resistor-coupled capacitor that directly participates in resonance. This capability enables deterministic assembly of nanocircuits with controlled symmetry and tunable nanogaps. The multilayer barrel scaffold yields a non-close-packed, symmetry-broken trimer with a magnetic resonance exhibiting a Q-factor of ∼19.2, exceeding values reported for comparable plasmonic clusters. Selective dye loading onto origami enables predictive light-molecule coupling, producing a 100-fold PRET enhancement in dimers over monomers. This approach provides a versatile route to designer optical resonances for nanophotonic applications.