Light-Harvesting Nanoparticle Core–Shell Clusters with Controllable Optical Output

Abstract

We used DNA self-assembly methods to fabricate a series of core–shell gold nanoparticle–DNA–colloidal quantum dot (AuNP–DNA–Qdot) nanoclusters with satellite-like architecture to modulate optical (photoluminescence) response. By varying the intercomponent distance through the DNA linker length designs, we demonstrate precise tuning of the plasmon–exciton interaction and the optical behavior of the nanoclusters from regimes characterized by photoluminescence quenching to photoluminescence enhancement. The combination of detailed X-ray scattering probing with photoluminescence intensity and lifetime studies revealed the relation between the cluster structure and its optical output. Compared to conventional light-harvesting systems like conjugated polymers and multichromophoric dendrimers, the proposed nanoclusters bring enhanced flexibility in controlling the optical behavior toward a desired application, and they can be regarded as controllable optical switches <i>via</i> the optically pumped color