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We propose a novel method for ultra-sensitive infrared (IR) vibrationalspectroscopy of molecules with nanoscale footprints by combining the tipenhancement of the scattering-type scanning near-field optical microscope(s-SNOM) and the plasmon enhancement of the breathing-mode (BM) plasmonresonances of graphene nanodisks (GNDs). To demonstrate that, we developed aquantitative model that is capable of computing accurately the s-SNOM signalsof nanoscale samples. With our modeling, we show that the s-SNOM tip caneffectively excite gate-tunable BM plasmonic resonances in GNDs with strongfield enhancement and sensitive dependence on the size of GND. Moreover, wedemonstrate that the intense electric field of tip-excited plasmonic BMs canstrongly enhance the IR vibrational modes of molecules. As a result, IRvibrational signatures of individual molecular particles with sizes down to 1-2nm can be readily observable by s-SNOM. Our study sheds light on futureultra-sensitive IR biosensing that takes advantage of both the tip and plasmonenhancement.

Tip-and plasmon-enhanced infrared nanoscopy for ultrasensitive molecular characterizations