Electron and Light Induced Stimulated Raman Spectroscopy for Nanoscale Molecular Mapping

We propose and theoretically analyze a new vibrational spectroscopy, termed electron- and light-induced stimulated Raman (ELISR) that combines the high spatial resolution of electron microscopy with the molecular specificity of surface-enhanced Raman spectroscopy. With ELISR, electron-beam excitation of plasmonic nanoparticles is utilized as a spectrally-broad but spatially-confined Stokes beam in the presence of a laser pump. ELISR promises simultaneous structural and chemical information with nanometer-scale resolution, without the need for advanced electron sources or monochromators.