Strong near-field light-matter interaction in plasmon-resonant tip-enhanced Raman scattering in indium nitride

TL;DR

This paper investigates the strong near-field Raman enhancement in tip-enhanced Raman scattering of indium nitride, revealing unique combinational modes and the role of surface charge accumulation in achieving resonance conditions.

Contribution

It demonstrates the occurrence of combinational Raman modes in InN during TERS and links the enhancement to surface charge accumulation enabling plasmon resonance.

Findings

Detection of near-field Raman modes not visible in far-field

Resonance condition between LSPs, SPPs, and surface charge oscillations

Large TERS signal enhancement due to surface charge accumulation

Abstract

We report a detailed study of the strong near-field Raman scattering enhancement which takes place in tip-enhanced Raman scattering (TERS) in indium nitride. In addition to the well-known first-order optical phonons of indium nitride, near-field Raman modes, not detectable in the far-field, appear when approaching the plasmonic probe. The frequencies of these modes coincide with calculated energies of second order combinational modes consisting of optical zone center phonons and acoustic phonons at the edge of the Brillouin zone. The appearance of strong combinational modes suggests that TERS in indium nitride represents a special case of Raman scattering in which a resonance condition on the nanometer scale is achieved between the localized surface plasmons (LSPs) and surface plasmon polaritons (SPPs) of the probe with the surface charge oscillation of the material. We suggest that the surface charge accumulation (SCA) in InN, which can render the surface a degenerate semiconductor, is the dominating reason for the unusually large enhancement of the TERS signal as compared to other inorganic semiconductors. Thus, the plasmon-resonant TERS (PR-TERS) process in InN makes this technique an excellent tool for defect characterization of indium-rich semiconductor heterostructures and nanostructures with high carrier concentrations.