(Invited) Multiphysics Model of the sSNOM Spectroscopy: Can Near-Field Probes Report the Spectrum of Nanomaterials?

Abstract

Last decade has been celebrated with a substantial increase of publications on imaging of nanomaterials with near-field probes. The latter include Tip-Enhanced Raman and/or Photoluminescence Spectroscopy (TERS/TEPL), various near-infrared (NIR) Atomic Force Microscopy (AFM) based methods, and several scattering Scanning Near-field optical methods (sSNOM). Using various coherent sources, often tunable in terms of excitation, these methods produce high spatial resolution images – near-field scanning maps, in terms of a pixel size claimed to be limited only by the size of the scanning tip.By design, TERS/TEPL detects a spectral response at each point of a map, which is, naively speaking, gives us a local probe of optical material properties within a single pixel (at the fixed excitation wavelength). NIR-AFM and sSNOM (leaving aside the FTIR mode) allow to obtain quasi-spectral information by tweaking the excitation. In this case, the collected (elastic) signal is restricted to the wavelength of the excitation.The essence of the near-field method is in breaking the laws of a plane-wave reflection from the sample, which requires a sub-wavelength separation between the tip and the sample and a strong enough near-field coupling between those. Still, it is routinely assumed that the tip is an “ideal probe” and its role is to “channel” the information about the local optical response to the detector. Up to date, little is known about the spectral response of the tip-sample system from the perspective of quantum physics.In this work, several aspects of the problem: mechanical motion of the scanning tip, electrodynamics of the excitation/scattered light, and quantum solid state description of the sample and the tip – are combined to obtain, within a simple model, a full picture of the near-field detection. The results, though not general and limited by the simplicity of model used for the sake of clarity of derivation, shed the light on the spectral response of a typical near-field microscope and describe effects, earlier called “artifacts”, as natural response for coupled tip-sample elementary excitations. Lastly, an application of the model for an analysis of spectra of nBN heteronanotubes (Y. Feng, et.al, ACS Nano 15, 5600, 2021) will be presented. Acknowledgement: This work has been partially supported by NSF MRSEC (DMR-2011839).Fig. 1. (left) Amplitude and phase of the near-field optical signal vs. the optical frequency: S(ω). (right) Same optical amplitude and phase vs. ω and the phase of mechanical motion of an AFM tip. Figure 1