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Chemical sensing methods based on surface polaritonic resonances stem from their intense near fields and resultant sensitivity to changes in local refractive index. Polar dielectric crystals (e.g., SiC, hBN) support surface phonon polaritons (SPhPs) from the mid-infrared to terahertz range with mode volumes and quality factors exceeding the best case scenario attained by plasmonic counterparts, making them strong candidates for resonant surface-enhanced infrared spectroscopy. We report on the behavior of SPhP resonances of SiC nanopillars following the incorporation of sub-nano- and nanometric coatings of Al2O3 and ZrO2 obtained by atomic layer deposition. Concurrent anomalous red- and blue-shifts of SPhP resonances were observed upon deposition of sub-nanometric Al2O3 films, with shift direction dictated by the mode position relative to the ordinary longitudinal optic phonon of Al2O3. These concurrent shifts, which are attributed to coupling to the Berreman mode of the Al2O3 layer, persist for thicker fi...

Sub-nanometer Thin Oxide Film Sensing with Localized Surface Phonon Polaritons