Colloidal Assembly of Au–Quantum Dot–Au Sandwiched Nanostructures with Strong Plasmon–Exciton Coupling

Strong plasmon–exciton coupling could occur in hybrid metal–dye/semiconductor nanostructures, where the fast energy exchange between plasmons and excitons leads to two new eigenmodes of the system, known as Rabi splitting. In experiments, strongly coupled nanosystems are difficult to obtain because they require some strict conditions, such as low plasmonic damping, small plasmon mode volume, and good spectral overlap. This work demonstrates strongly coupled metal–semiconductor nanostructures can be constructed using colloidal assembly. Specifically, sandwiched Au–quantum dot–Au nanostructures were created through the assembly of Au nanoparticles and colloidal quantum dots (QDs). The sizes of the QDs and the assembly conditions were varied to control the mode volume of the plasmonic cavity formed between the two Au nanoparticles. With a decreased gap size, Rabi splitting was observed in both dark-field scattering and fluorescence spectra of single Au–QD–Au nanostructures. Theoretical simulations revealed that the strong coupling occurred between the excitons and the octupolar plasmon modes.