All-Optical Imaging of Gold Nanoparticle Geometry Using Super-Resolution Microscopy

[Image: see text] We demonstrate the all-optical reconstruction of gold nanoparticle geometry using super-resolution microscopy. We employ DNA-PAINT to get exquisite control over the (un)binding kinetics by the number of complementary bases and salt concentration, leading to localization accuracies of ∼5 nm. We employ a dye with an emission spectrum strongly blue-shifted from the plasmon resonance to minimize mislocalization due to plasmon-fluorophore coupling. We correlate the all-optical reconstructions with atomic force microscopy images and find that reconstructed dimensions deviate by no more than ∼10%. Numerical modeling shows that this deviation is determined by the number of events per particle, and the signal-to-background ratio in our measurement. We further find good agreement between the reconstructed orientation and aspect ratio of the particles and single-particle scattering spectroscopy. This method may provide an approach to all-optically image the geometry of single particles in confined spaces such as microfluidic circuits and biological cells, where access with electron beams or tip-based probes is prohibited.