One of the major challenges in nanophotonics is the direct measurement of the interaction of a nanostructure with a single fluorescent emitter at the nanometer level. Several approaches developed to this aim can be found in the literature. Recently, single molecule localization imaging, traditionally used for the study of biological samples, entered the nanophotonics realm opening new horizons. We report on the development of single-molecule fluorescence lifetime imaging microscopy (sm-FLIM), an innovative approach enabling the simultaneous measurement of the lifetime and the intensity of single-molecules densely labeling a nanostructured sample, with a field of view of 10 µm2 , a spatial resolution of approximately 14 nm and a temporal resolution of approximately 50 ps. smFLIM enabled us to image, at the single molecule level, the Local Density of Optical States (LDOS, which is related to the inverse of the fluorescence lifetime) of dielectric nanoantennas and periodic arrays of hollow truncated plasmonic nanocones.
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.
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