Polarization-Resolved Electron Energy Gain Nanospectroscopy With Phase-Structured Electron Beams

Free-electron-based measurements in scanning transmission electron microscopes (STEMs) reveal valuable information on the broadband spectral responses of nanoscale systems with deeply subdiffraction limited spatial resolution. Leveraging recent advances in manipulating the spatial phase profile of the transverse electron wavefront, we theoretically describe interactions between the electron probe and optically stimulated nanophotonic targets in which the probe gains energy while simultaneously transitioning between transverse states with distinct phase profiles. Exploiting the selection rules governing such transitions, we propose phase-shaped electron energy gain nanospectroscopy for probing the 3D polarization-resolved response field of an optically excited target with nanoscale spatial resolution. Considering ongoing instrumental developments, polarized generalizations of STEM electron energy loss and gain measurements hold the potential to become powerful tools for fundamental studies of quantum materials and their interaction with nearby nanostructures supporting localized surface plasmon or phonon polaritons as well as for noninvasive imaging and nanoscale 3D field tomography.