Nanostructure-induced distortion in single-emitter microscopy

Abstract: Single-emitter microscopy has emerged as a promising method of imaging nanostructures with nanoscale resolution. This technique uses the centroid position of an emitters far-field radiation pattern to infer its position to a precision that is far below the diffraction limit. However, nanostructures composed of high-dielectric materials such as noble metals can distort the far-field radiation pattern. Nanoparticles also exhibit a more complex range of distortions, because in addition to introducing a high dielectric surface, they also act as efficient scatterers. Thus, the distortion effects of nanoparticles in single-emitter microscopy remains poorly understood. Here we demonstrate that metallic nanoparticles can significantly distort the accuracy of single-emitter imaging at distances exceeding 300 nm. We use a single quantum dot to probe both the magnitude and the direction of the metallic nanoparticle-induced imaging distortion and show that the diffraction spot of the quantum dot can shift by more than 35 nm. The centroid position of the emitter generally shifts away from the nanoparticle position, in contradiction to the conventional wisdom that the nanoparticle is a scattering object that will pull in the diffraction spot of the emitter towards its center. These results suggest that dielectric distortion of the emission pattern dominates over scattering. We also show that by monitoring the distortion of the quantum dot diffraction spot we can obtain high-resolution spatial images of the nanoparticle, providing a new method for performing highly precise, sub-diffraction spatial imaging. These results provide a better understanding of the complex near-field coupling between emitters and nanostructures, and open up new opportunities to perform super-resolution microscopy with higher accuracy.