Probing lattice vibration of alkali halide crystals by broadband terahertz spectroscopy

Terahertz spectral features of alkali halide crystals were studied with the combination of broadband terahertz time-domain spectroscopy and the solid-state-based density functional theory calculations. To understand the particular modes of the observed terahertz features of the alkali halide crystals, the resonant modes of KCl and CsCl were analyzed using face-centered cubic and body-centered cubic lattice models, respectively. The results show that the characteristic terahertz absorption peaks could be assigned to the lattice vibration of the ionic crystals. Furthermore, the terahertz responses of a series of alkali halides were recorded, and obvious absorption peaks were observed in each salt in the frequency region below 8.5 THz. What is more interestingly is that the frequencies of these observed peaks are red-shifted with the increases of the mass and radius of the ions. This correlation between the resonant frequency of the lattice vibration, the reduced atomic mass, and the equilibrium distance between the ions agrees well with the harmonic oscillator model.