Dynamics of Strong Coupling between CdSe Quantum Dots and Surface Plasmon Polaritons in Subwavelength Hole Array.

We have investigated the strong coupling interaction between excitons of CdSe quantum dots (QDs) and surface plasmon polaritons (SPPs) of gold nanohole array by steady-state spectroscopic method and transient absorption measurements. Numerical and experimental steady-state measurements demonstrate that the SPP-QD system can indeed undergo strong coupling, characterized by a Rabi splitting up to 220 meV. In particular, it is found that in the transient absorption spectra, under resonant excitation, the 1S transition bleaching band from uncoupled CdSe QDs is completely separated into two distinctive bleaching bands, remarkably fingerprinting the hybrid SPP-QD state. It was also found that the lifetime of these hybrid bands is just slightly shorter than the lifetime of bare CdSe QDs, possibly caused by the phonon bottleneck effect due to the large Rabi splitting. These results could open a new avenue toward the development of novel nanoplasmon devices with strong SPP-QD interaction.