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The Raman effect -- inelastic scattering of light by lattice vibrations(phonons) -- produces an optical response closely tied to a material's crystalstructure. Here we show that resonant optical excitation of IR and Ramanphonons gives rise to a Raman scattering effect that can induce giant shifts tothe refractive index and induce new optical constants that are forbidden in theequilibrium crystal structure. We complete the description of light-matterinteractions mediated by coupled IR and Raman phonons in crystalline insulators-- currently the focus of numerous experiments aiming to dynamically controlmaterial properties -- by including a forgotten pathway through the nonlinearlattice polarizability. Our work expands the toolset for control anddevelopment of new optical technologies by revealing that the absorption oflight within the terahertz gap can enable control of optical properties ofmaterials over a broad frequency range.

Ultrafast control of material optical properties via the infrared resonant Raman effect