Surface Phonon Polariton Ellipsometry

Surface phonon polaritons (SPhPs) have become a key ingredient for infrared nanophotonics owing to their long lifetimes and the large number of polar dielectric crystals supporting them. While these evanescent modes have been thoroughly characterized by near-field mapping or far-field intensity measurements over the past decade, far-field optical experiments also providing phase information are less common. In this Article, we study surface phonon polaritons at the gallium phosphide (GaP)–air interface in the momentum domain using the Otto-type prism coupling geometry. We combine this method with spectroscopic ellipsometry to obtain both amplitude and phase information on the reflected waves across the entire reststrahlen band of GaP. By adjusting the prism–sample air gap width, we systematically study the dependence of the ellipsometry parameters on the optical coupling efficiency. In particular, we show that the combined observation of both ellipsometry parameters, amplitude and phase, provides a powerful tool for the detection of SPhPs, even in the presence of high optical losses. Finally, we theoretically study how surface phonon polariton ellipsometry can reveal the emergence of vibrational strong coupling through changes in the topology of their complex plane trajectories, opening up a new perspective on light–matter coupling.