When driven at infrared resonances, crystals possess giant Raman scattering susceptibilities due to nonlinear lattice coupling in the polarizability. A first-principles study of SrTiO3 reveals Stokes and anti-Stokes peaks in the cubic susceptibility with values >10^(-15) m^2/V^2, and large values of chi^(3) representing cross-phase and cross-amplitude modulation that persist from THz to visible frequencies. This implies a new route for achieving strong nonlinear frequency conversion in the infrared over short length scales, and a route for strong light-driven control of material optical properties on ultrafast timescales covering a hyperspectral range. We additionally discuss implications for non-centrosymmetric materials such as LiNbO3.
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