Abstract
Two-dimensional (2D) multiferroic materials with the coexistence of electric and spin polarization offer a tantalizing potential for high-density multistate data storage. However, intrinsic 2D multiferroic semiconductors with high thermal stability are still rare to date. Here, we propose a new mechanism of single-phase multiferroicity. Based on first-principles calculations, we predicted that in a CrO3 monolayer, the unconventional distortion of the square antiprismatic crystal field on Cr-d orbitals will induce an in-plane electric polarization, making this material a single-phase multiferroic semiconductor. Importantly, the magnetic Curie temperature is estimated to be ∼220 K, which is quite high as compared to those of the recently reported 2D ferromagnetic and multiferroic semiconductors. Moreover, both ferroelectric and antiferroelectric phases are observed, providing opportunities for electrical control of magnetism and energy storage and conversion applications. These findings provide a comprehensive understanding of the magnetic and electric behavior in 2D multiferroics and will motivate further research on the application of related 2D electromagnetics and spintronics.
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