Spontaneous and Stimulated Electron-Photon Interactions in Nanoscale Plasmonic Near Fields

Abstract: We demonstrate spatially-resolved measurements of spontaneous and stimulated electron-photon interactions in nanoscale optical near fields using electron energy-loss spectroscopy (EELS), cathodoluminescence spectroscopy (CL), and photon-induced near-field electron microscopy (PINEM). Specifically, we study resonant surface plasmon modes that are tightly confined to the tip apexes of an Au nanostar, enabling a direct correlation of EELS, CL, and PINEM on the same physical structure at the nanometer length scale. Complemented by numerical electromagnetic boundary-element method calculations, we discuss the spontaneous and stimulated electron-photon interaction strength and spatial dependence of our EELS, CL and PINEM distributions. We demonstrate that in the limit of an isolated tip mode, spatial variations in the electron-near field coupling are fully determined by the modal electric field profile, irrespective of the spontaneous (in EELS and CL) or stimulated nature (in PINEM) of the process. Yet we show that coupling to the tip modes crucially depends on the incident electron energy with a maximum at a few keV, depending on the proximity of the interaction to the tip apex. Our results provide elementary insights into spontaneous and stimulated electron-light-matter interactions at the nanoscale that have key implications for research on (quantum) coherent optical phenomena in electron microscopy.