Second-order Jahn–Teller effect induced high-temperature ferroelectricity in two-dimensional NbO2X (X = I, Br)

Abstract

Based on the first-principles calculations, we investigated the ferroelectric properties of two-dimensional (2D) materials NbO₂X (X = I, Br). Our cleavage energy analysis shows that exfoliating one NbO₂I monolayer from its existing bulk counterpart is feasible. The phonon spectrum and molecular dynamics simulations confirm the dynamic and thermal stability of the monolayer structures for both NbO₂I and NbO₂Br. Total energy calculations show that the ferroelectric phase is the ground state for both materials, with the calculated in-plane ferroelectric polarizations being 384.5 pC m⁻¹ and 375.2 pC m⁻¹ for monolayers NbO₂I and NbO₂Br, respectively. Moreover, the intrinsic Curie temperature T_C of monolayer NbO₂I (NbO₂Br) is as high as 1700 K (1500 K) from Monte Carlo simulation. Furthermore, with the orbital selective external potential method, the origin of ferroelectricity in NbO₂X is revealed as the second-order Jahn–Teller effect. Our findings suggest that monolayers NbO₂I and NbO₂Br are promising candidate materials for practical ferroelectric applications.