Nanometer-Scale Spatial and Spectral Mapping of Exciton Polaritons in Structured Plasmonic Cavities

Exciton polaritons (EPs) are ubiquitous light-matter excitations under intense investigation as test beds of fundamental physics and as components for all-optical computing. Owing to their unique attributes and facile experimental tunability, EPs potentially enable strong nonlinearities, condensation, and superfluidity at room temperature. However, the diffraction limit of light and the momentum content of fast electron probes preclude the characterization of EPs in nanoscale structured cavities exhibiting energy-momentum dispersion. Here we present fully relativistic analytical theory and companion numerical simulations showing that these limitations can be overcome to measure EPs in periodic nanophotonic cavities on their natural energy, momentum, and length scales via lattice electron energy gain spectroscopy. With the combined high momentum resolution of light and nanoscale spatial resolution of focused electron beams, lattice electron energy gain spectroscopy can expose deeply subwavelength EP features using currently available monochromated, aberration-corrected scanning transmission electron microscopes.