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High-order nonlinear light-matter interactions in gases enable generation ofx-ray and attosecond light pulses, metrology, and spectroscopy. Opticalnonlinearities in solid-state materials are particularly interesting forcombining optical and electronic functions for high-bandwidth informationprocessing. Third-order nonlinear optical processes in silicon have been usedto process optical signals with greater than 1 GHz bandwidths. Fundamentalphysical processes for a Si-based optical modulator in the THz bandwidth range,however, have not yet been explored. Here we demonstrate ultrafast phononicmodulation of the optical index of Si by irradiation with intense few-cyclefemtosecond pulses. The anisotropic reflectivity modulation by the resonantRaman susceptibility at the fundamental frequency of the longitudinal optical(LO) phonon of Si (15.6 THz) generates a frequency comb up to 7th-order. Alloptical >100 THz frequency comb generation is realized by harnessing thecoherent atomic motion of the Si crystalline lattice at its highest mechanicalfrequency.

Frequency comb generation at THz frequencies by coherent phonon excitation in Si