Ferroelectricity, nonlinear dynamics, and relaxation effects in monoclinic Sn2P2S6

An ab initio-based model of the temperature-induced ferroelectric phase transition in Sn2P2S6 (SPS) as a prototype of an unconventional ferroelectric is developed. The order parameter in SPS is found as the valley line on a total-energy surface of the zone-center fully symmetrical A(g) and polar B-u distortions. Significant nonlinear coupling between order parameter and strain is observed. Monte Carlo simulations describe the additional low-temperature rearrangement in polar structure, which appears in domain boundaries, and describe the relaxation phenomena near the ferroelectric phase transition.