The ultrafast dynamics of electrons and phonons excited by femtosecond light pulses in ferroelectric semiconductor Sn 2 P 2 S 6 is investigated using the optical pump-probe technique. It is demonstrated that a soft mode can be excited in this ferroelectric in the vicinity of the phase transition initiated by laser radiation.

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Objectives. Advances in laser physics over the last decade have led to the creation of sources of single-period electromagnetic pulses having a duration of about 1 ps, corresponding to the terahertz (THz) frequency range and a field amplitude of several tens of MV/cm. This allows the electrode-free application of an electric field to a ferroelectric for observing not only the excitation of coherent phonons, but also ultrafast (at the sub-picosecond timescale) dynamic polarization switching. To detect polarization switching, a pump-probe technique is used in which a THz pulse is used with an optical probe. Since its intensity is proportional to the square of the polarization, the signal of the optical second harmonic is used to measure polarization switching under the action of a THz pulse. To evaluate switching efficiency, both linear (refractive index and absorption coefficient) and non-linear optical characteristics (quadratic and cubic susceptibilities) are required. For any application of ferroelectric crystals in the THz range, knowledge of the relevant linear optical characteristics is also necessary.Methods. The technique of THz spectroscopy in the time domain was used; here, a picosecond THz pulse transmitted through the crystal is recorded by strobing the detector with a femtosecond optical pulse. The THz-induced dynamics of the order parameter in a ferroelectric was studied by detecting the intensity of a nonlinear optical signal at the frequency of the second optical harmonic.Results. The transmission of a THz wave and the intensity of second harmonic generation on a lead germanate crystal doped with silicon in the time and spectral domains were measured. On this basis, the absorption coefficient dispersion and cubic nonlinear susceptibility were calculated in the range of 0.5-2.0 THz. The presence of a region of fundamental absorption near the phonon modes was confirmed along with a resonant enhancement of the cubic nonlinear susceptibility for two phonon modes Ω1 = 1.3 THz and Ω2 = 2.0 THz.Conclusions. The proposed technique is effective for analyzing the dispersion of the optical characteristics of ferroelectric crystals. The significantly improved spectral resolution (0.1 THz) increases the accuracy of determining nonlinear susceptibility due to the detailed analysis of the linear and nonlinear contributions to the second harmonic intensity.