Real-time observation of phonon-polariton dynamics in ferroelectric LiNbO3 in time-frequency space

We demonstrate the real-time observation of phonon-polariton propagation in ferroelectric LiNbO3 using a single-shot spectroscopic setup that employs an echelon mirror. The echelon mirror provides a spatially encoded time delay for the probe pulse; therefore, the ultrafast transient behavior of materials can be detected on a single-shot basis. Using optical Kerr gate apparatus, forward and backward propagating E-mode phonon-polaritons were simultaneously induced via an impulsive stimulated Raman scattering process, and subsequently, their dynamics were readily mapped in time-frequency space using heterodyne detection. The two phonon-polaritons appeared on opposite sides of the central probe wavelength and were symmetrically imaged against the ordinary and extraordinary probe lights. By taking into account coupling of the lowest E-mode phonon-polariton to a low-frequency relaxational mode, not only the phonon-polariton dispersion but also the wavevector dependence of the damping rate was unveiled and quantitatively evaluated.