We observe strongly anisotropic third-harmonic generation mediated by resonant sum-frequency driving of Raman-active phonons with terahertz light, extending light-induced dual control of structural and optical properties in solids. Either strong enhancement or strong suppression of the third harmonic can be achieved, covering six orders of magnitude, a result of interference between purely electronic and phonon-mediated contributions to the polarization field. These findings enrich capabilities for tailoring nonlinear optics via phononics and for the spectroscopy of crystalline structural dynamics.
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Zheng et al. (2024) studied this question.
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