Plasmon dephasing time and optical field enhancement in a plasmonic nanobowl substrate studied by scanning near-field optical microscopy

Plasmonic substrates have been extensively investigated due to their potential applications in fluorescence microscopy, chemical sensing, and photochemical reactions. The optical properties of the substrate depend on the spatial and temporal features of the plasmon excited. Hence, the ability to directly visualize plasmon dynamics is crucial. In this study, we investigated the spatial and temporal properties of plasmon excitation in a plasmonic nanobowl substrate consisting of a periodic hexagonal array of nanoscale bowl-like structures developed with self-assembly. Near-field transmission imaging revealed that multiple plasmon resonance bands are observed from visible to near-infrared spectral region, and the optical contrast of the image is dependent on the observed band. Near-field two-photon photoluminescence microscopy revealed that the probability of excitation inside each nanoscale bowl-like structure is greater than that in the surrounding area. Near-field time-resolved imaging revealed that the nanobowl substrate exhibited a substantially long plasmon dephasing time, exceeding 12 fs. Based on the spectral features of the near-field and far-field spectra, we found that optically dark plasmon mode is excited by the near-field illumination and only partly contributes to the long dephasing time observed. This fact indicates that the dephasing time is extended by some other mechanism in the periodic substrate. We revealed from this study that the enhanced optical fields induced in the nanobowl structure originate from the photosynergetic effect of the cavity mode and plasmon mode excited.