Single-molecule localization to imaging the LDOS modification by an array of plasmonic hollow conical nanopillars

Abstract

We study the modification of fluorescence emission and decay rate of single fluorescent molecules in the near field of a periodic plasmonic nanostructure formed by a square lattice of Au hollow conical pillars with a periodicity of 250 nm. We perform nanometer-resolved imaging of the LDOS by simultaneously mapping the position and the decay rate of photoactivatable single-molecules with a novel super-resolved microscopy approach which enables multiplexed and super-resolved fluorescence lifetime imaging at the single-molecule level (smFLIM) with a field of view of ~10 µm2. We observe the LDOS modification of such optically rich material at different illumination conditions and we measure a large Purcell factor enhancement which increases for oblique illumination of the nanostructure.