Single-molecule-resolution ultrafast near-field optical microscopy via plasmon lifetime extension.

A recent study shows that: when a long lifetime particle is positioned near a plasmonic metal nanoparticle, lifetime of plasmon oscillations extends, but, "only" near that long-life particle [PRB 101, 035416 (2020)]. Here, we show that this phenomenon can be utilized for ultrahigh (single-molecule) resolution ultrafast apertureless (scattering) SNOM applications. We use the exact solutions of 3D Maxwell equations. We illuminate a metal-coated silicon tip, a quantum emitter (QE) placed on the tip apex, with a femtosecond laser. The induced near-field in the apex decays rapidly except in the vicinity of the sub-nm-sized QE. Thus, the resolution becomes solely limited by the size of the QE. As positioning of a QE on the tip apex is challenging, we propose the use of a newly-discovered phenomenon; stress-induced defect formation in 2D materials. When a monolayer, e.g., transition metal dichalcogenide (TMD) is transferred to the AFM tip, the tip indentation of 2D TMD originates a defect-center located right at the sharpest point of the tip; that is exactly at its apex. Moreover, the resonance of the defect is tunable via a voltage applied to the tip. Our method can equally be used for background-noise-free nonlinear imaging and for facilitating single-molecule-size chemical manipulation.