Optical scattering imaging with sub-nanometer precision based on position-ultra-sensitive giant Lamb shift

TL;DR

This paper introduces a highly sensitive optical localization method using giant Lamb shift-induced scattering spectrum shifts, enabling sub-nanometer precision in quantum emitter positioning without fluorescence quenching.

Contribution

It proposes a novel microscopy technique based on scattering spectrum shifts caused by giant Lamb shifts, avoiding fluorescence quenching and broadening application scope.

Findings

Achieves sub-nanometer localization precision.

Detects Lamb shift via scattering spectrum dip shifts.

Works without placing emitters inside plasmonic cavities.

Abstract

The Lamb shift of a quantum emitter very close to a plasmonic nanostructure, mainly induced by the higher-order plasmonic dark modes, can be three or more orders of magnitude larger than that in the free space and it is ultra-sensitive to the emitter position and polarization. We show that this giant Lamb shift can be sensitively observed from the scattering spectrum dip shift of coupled system when the plasmonic nanoparticle or tip scans through the emitter. Based on these observations, we propose an optical localization and polarization microscopy scheme with sub-nanometer precision for a quantum emitter via detecting the scattering spectrum instead of fluorescence. Our method is free of fluorescence quenching problem and it is relatively easier to be implemented in the plasmon-emitter coupling system. Moreover, the sample in our method does not need to be placed inside a plasmonic picocavity to enhance the radiative fluorescence rate and it also works even if the quantum emitter is slightly below a dielectric surface which can bring about broader applications in various fields, such as physics, chemistry, medicine, life science and materials science.