Plasmon point spread functions: How do we model plasmon-mediated emission processes?

Abstract

A major challenge with studying plasmon-mediated emission events is the small size of plasmonic nanoparticles relative to the wavelength of light. Objects smaller than roughly half the wavelength of light will appear as diffraction-limited spots in far-field optical images, presenting a significant experimental challenge for studying plasmonic processes on the nanoscale. Super-resolution imaging has recently been applied to plasmonic nanosystems and allows plasmon-mediated emission to be resolved on the order of ∼5 nm. In super-resolution imaging, a diffraction-limited spot is fit to some model function in order to calculate the position of the emission centroid, which represents the location of the emitter. However, the accuracy of the centroid position strongly depends on how well the fitting function describes the data. This Perspective discusses the commonly used two-dimensional Gaussian fitting function applied to super-resolution imaging of plasmon-mediated emission, then introduces an alternative model based on dipole point spread functions. The two fitting models are compared and contrasted for super-resolution imaging of nanoparticle scattering/luminescence, surface-enhanced Raman scattering, and surface-enhanced fluorescence.