Spectroscopic and Interferometric Sum‐Frequency Imaging of Strongly Coupled Phonon Polaritons in SiC Metasurfaces

Phonon polaritons enable waveguiding and localization of infrared light with extreme confinement and low losses. The spatial propagation and spectral resonances of such polaritons are usually probed with complementary techniques such as near‐field optical microscopy and far‐field reflection spectroscopy. Here, infrared‐visible sum‐frequency spectro‐microscopy is introduced as a tool for spectroscopic imaging of phonon polaritons. The technique simultaneously provides sub‐wavelength spatial resolution and highly‐resolved spectral resonance information. This is implemented by resonantly exciting polaritons using a tunable infrared laser and wide‐field microscopic detection of the upconverted light. The technique is employed to image hybridization and strong coupling of localized and propagating surface phonon polaritons in a metasurface of SiC micropillars. Spectro‐microscopy allows to measure the polariton dispersion simultaneously in momentum space by angle‐dependent resonance imaging, and in real space by polariton interferometry. Notably, it is possible to directly image how strong coupling affects the spatial localization of polaritons, inaccessible with conventional spectroscopic techniques. The formation of edge states is observed at excitation frequencies where strong coupling prevents polariton propagation into the metasurface. The technique is applicable to the wide range of polaritonic materials with broken inversion symmetry and can be used as a fast and non‐perturbative tool to image polariton hybridization and propagation. A non‐linear technique of infrared + visible sum‐frequency spectro‐microscopy is introduced to image phonon polaritons in SiC metasurfaces. This approach allows for access to both the spatial propagation and spectral dispersion of the polaritons with sub‐wavelength spatial resolution. The hybridization and strong coupling of propagating (SPhP) and localized (LSPhP) phonon polaritons and the activation of polaritonic edge states are observed.