Ultra-high resolution aSNOM imaging at off-resonant wavelengths (1807.07863v3)

Abstract: An atomic force microscope~(AFM) tip, with a few nm-thick noble metal coating, gives rise to strong electric-field at the near-field of tip apex, i.e. hot spot, when illuminated with a beam of light linearly polarized in the axial direction. This strong near-field enables resolving molecular landscape or nano-scale defects on crystal surfaces in apertureless scanning near field optical microscopy or tip enhanced Raman spectroscopy applications. However, strong near fields appear only at certain illumination wavelengths at which material and geometry dependent plasmon resonances take place. Once the metal coated tip is manufactured, optimal operation wavelength remains fixed since the material and geometry of the tip apex remains fixed. Here, we show for the first time a method which renders an AFM tip useful at wavelengths off-resonant to its plasmon resonances. The technique relies on decoration of the tip with appropriate auxiliary molecules. For instance, a tip originally bearing a plasmon resonance at $\lambda_{\rm p}=581$ nm can be effectively operated off-resonantly at $\lambda_{\rm exc}=532$ nm, when it is decorated by an appropriate auxiliary molecule. Furthermore, the near-field is found to be strongest just below the auxiliary molecule which enables a single-molecule-size ultra-high spatial resolution imaging. We demonstrate the phenomenon with exact solutions of 3D Maxwell equations. We also show why such an enhancement takes place.