Defocused imaging-based quantification of plasmon-induced distortion of single emitter emission.

Optical properties of single emitters can be significantly improved through the interaction with plasmonic structures, leading to enhanced sensing and imaging capabilities. In turn, single emitters can act as sensitive probes of the local electromagnetic field surrounding plasmonic structures, furnishing fundamental insights into their physics and guiding the design of novel plasmonic devices. However, the interaction of emitters in the proximity to a plasmonic nanostructure causes distortion, which hinders precise estimation of position and polarization state and is one of the reasons why detection and quantification of molecular processes yet remain fundamentally challenging in this era of super-resolution. Here, we investigate axially defocused images of a single fluorescent emitter near metallic nanostructure, which encode emitter positions and can be acquired in the far-field with high sensitivity, while analyzing the images with pattern matching algorithm to explore emitter-localized surface plasmon interaction and retrieve information regarding emitter positions. Significant distortion in defocused images of fluorescent beads and quantum dots near nanostructure was observed and analyzed by pattern matching and finite-difference time-domain methods, which revealed that the distortion arises from the emitter interaction with nanostructure. Pattern matching algorithm was also adopted to estimate the lateral positions of a dipole that models an emitter utilizing the distorted defocused images and achieved improvement by more than 3 times over conventional diffraction-limited localization methods. The improvement by defocused imaging is expected to provide a way of enhancing reliability when using plasmonic nanostructure and diversifying strategies for various imaging and sensing modalities.