Anharmonic phonon-polariton dynamics in ferroelectric LiNbO3 studied with single-shot pump-probe imaging spectroscopy

We demonstrate that single-shot pump-probe imaging spectroscopy with an echelon mirror enables us to disclose the ferroelectric phonon-polariton dynamics across a wide temperature range from 10 K to 375 K while avoiding the photorefractive effects that appear prominently at low temperatures. The E-mode phonon-polaritons corresponding to the two transverse optical modes, TO1 and TO3, up to ∼7 THz were induced in LiNbO3 through an impulsive stimulated Raman scattering process. Subsequently, using single-shot pump-probe imaging spectroscopy over a minimal cumulative time, we successfully visualized the phonon-polariton dynamics in time-wavelength space even at low temperatures. We found that the phase-matching condition significantly affected the observed temperature-dependent phonon-polariton frequency shift. The anharmonicity of the TO1 and TO3 modes was then evaluated based on an anharmonic model involving higher-order interactions with acoustic phonons while eliminating the influence of the frequency shift due to the phase-matching condition. The observed wavenumber-dependent damping rate was analyzed by considering the bilinear coupling of the TO1 or TO3 modes with the thermally activated relaxation mode. We found that the phonon-polariton with a higher frequency and wavenumber had a higher damping rate at high temperatures because of its frequent interaction with the thermally activated relaxation mode and acoustic phonons. The TO3 mode displayed greater bilinear coupling than the TO1 mode, which may also have contributed to the observed high damping rate. Thus, using our unique single-shot spectroscopy technique, we could reveal the overall anharmonic characteristics of the E-mode phonon-polaritons arising from both the acoustic phonons and the relaxation mode.journal articl

Terahertz-field-induced carrier generation in Bi1−xSbx Dirac electron systems

Terahertz-field-induced carrier generation processes were investigated in Dirac electron systems, single-crystalline bismuth antimony alloy thin films (Bi1−xSbx; 0≤x≤0.16). This investigation was performed by precisely tuning, via the substituent ratio x, the band structure of the films from that associated with a semimetal to that characteristic of a narrow-gap semiconductor. Terahertz-field-induced absorption was clearly observed within a few picoseconds after the terahertz pump-pulse illumination of Bi1−xSbx semimetal and semiconductor samples. The field-strength dependence of the induced absorption was compared with the calculated Zener tunneling probability in the Dirac-like band dispersion. Through this comparison, the mechanism of the induced absorption was attributed to the carrier generation via the terahertz-field-induced Zener tunneling. The tunneling occurred in subpicosecond timescales even at room temperature, demonstrating that Bi1−xSbx thin films are promising for future high-speed electronics and the investigation of universal ultrafast tunneling dynamics.journal articl