Spatial Variations in Femtosecond Field Dynamics within a Plasmonic Nanoresonator Mode

Nano Lett. 2019 Jul 10;19(7):4651-4658. doi: 10.1021/acs.nanolett.9b01672. Epub 2019 Jun 17.

Abstract

Plasmonic resonators can be designed to support spectrally well-separated discrete modes. The associated characteristic spatial patterns of intense electromagnetic hot-spots can be exploited to enhance light-matter interaction. Here, we study the local field dynamics of individual hot-spots within a nanoslit resonator by detecting characteristic changes of the photoelectron emission signal on a scale of ∼12 nm using time-resolved photoemission electron microscopy (TR-PEEM) and by excitation with the output from a 20 fs, 1 MHz noncollinear optical parametric amplifier (NOPA). Surprisingly, we detect apparent spatial variations of the Q-factor and resonance frequency that are commonly considered to be global properties for a single mode. By using the concept of quasinormal modes we explain these local differences by crosstalk of adjacent resonator modes. Our findings are important in view of time-domain studies of plasmon-mediated strong light-matter coupling at ambient conditions.

Keywords: Plasmonics; cavity; quasinormal modes; time-resolved PEEM.