Correlative electron and light spectroscopy of strongly-coupled mid-infrared plasmon and phonon polaritons

Abstract: The ability to control and modify infrared excitations in condensed matter is of both fundamental and application interests. Here we explore a system supporting low-energy excitations, in particular, mid-infrared localized plasmon modes and phonon polaritons that are tuned to be strongly coupled. We study the coupled modes by using far-field infrared spectroscopy, state-of-the-art monochromated electron energy-loss spectroscopy, numerical simulations and analytical modeling. We demonstrate that the electron probe facilitates a precise characterization of polaritons constituting the coupled system, and enables an active control over the coupling and the resulting sample response both in frequency and space. Our work establishes a rigorous description of the spectral features observed in light- and localized electron-based spectroscopies, which can be extended to analogous optical systems with applications in heat management, and electromagnetic field concentration or nanofocusing.