Anharmonic stabilization of ferrielectricity in CuInP2Se6

Abstract

Using first-principles calculations and group-theory-based models, we study the stabilization of ferrielectricity (FiE) in CuInP2Se6. We find that the FiE ground state is stabilized by a large anharmonic coupling between the polar mode and a fully symmetric Raman-active mode. Our results open possibilities for controlling the single-step switching barrier for polarization by tuning the Raman-active mode. We discuss the implications of our findings in the context of designing next-generation optoelectronic devices that can overcome the voltage-time dilemma.