  We propose and theoretically analyze a new vibrational spectroscopy, termed
electron- and light-induced stimulated Raman (ELISR) scattering, that combines
the high spatial resolution of electron microscopy with the molecular
sensitivity of surface-enhanced Raman spectroscopy. With ELISR, electron-beam
excitation of plasmonic nanoparticles is utilized as a spectrally-broadband but
spatially-confined Stokes beam in the presence of a diffraction-limited pump
laser. To characterize this technique, we develop a numerical model and conduct
full-field electromagnetic simulations to investigate two distinct nanoparticle
geometries, nanorods and nanospheres, coated with a Raman-active material. Our
results show the significant ($10^6$-$10^7$) stimulated Raman enhancement that
is achieved with dual electron and optical excitation of these nanoparticle
geometries. Importantly, the spatial resolution of this vibrational
spectroscopy for electron microscopy is solely determined by the nanoparticle
geometry and the plasmon mode volume. Our results highlight the promise of
ELISR for simultaneous high-resolution electron microscopy with
sub-diffraction-limited Raman spectroscopy, complementing advances in
superresolution microscopy, correlated light and electron microscopy, and
vibrational electron energy loss spectroscopy.
