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A recent study shows that: when a long lifetime particle is positioned near aplasmonic metal nanoparticle, lifetime of plasmon oscillations extends, but,"only" near that long-life particle [PRB 101, 035416 (2020)]. Here, we showthat this phenomenon can be utilized for ultrahigh (single-molecule) resolutionultrafast apertureless (scattering) SNOM applications. We use the exactsolutions of 3D Maxwell equations. We illuminate a metal-coated silicon tip, aquantum emitter (QE) placed on the tip apex, with a femtosecond laser. Theinduced near-field in the apex decays rapidly except in the vicinity of thesub-nm-sized QE. Thus, the resolution becomes solely limited by the size of theQE. As positioning of a QE on the tip apex is challenging, we propose the useof a newly-discovered phenomenon; stress-induced defect formation in 2Dmaterials. When a monolayer, e.g., transition metal dichalcogenide (TMD) istransferred to the AFM tip, the tip indentation of 2D TMD originates adefect-center located right at the sharpest point of the tip; that is exactlyat its apex. Moreover, the resonance of the defect is tunable via a voltageapplied to the tip. Our method can equally be used for background-noise-freenonlinear imaging and for facilitating single-molecule-size chemicalmanipulation.

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