Distorted Monolayer ReS₂ with Low-Magnetic-Field Controlled Magnetoelectricity

Two dimensional (2D) materials possessing ferroelectric/ferromagnetic orders and especially low-magnetic-field controlled magnetoelectricity have great promise in spintronics and multistate data storage. However, ferroelectric and magnetoelectric (ME) dipoles in the atom-thick 2D materials are difficult to be realized due to structural inversion symmetry, thermal actuation, and depolarized field. To overcome these difficulties, the monolayer structure must possess an in-plane inversion asymmetry in order to provide out-of-plane ferroelectric polarization. Herein, crystal chemistry is adopted to engineer specific atomic displacement in monolayer ReS2 to change the crystal symmetry to induce out-of-plane ferroelectric polarization at room temperature. The cationic Re vacancy in the atom-displaced ReS2 monolayer causes spin polarization of two immediate neighbor sulfur atoms to generate magnetic ordering, and the ferroelectric distortion near the Re vacancy locally tunes the ferromagnetic order thereby triggering low-magnetic-field controlled ME polarization at about 28 K. As a result, 2D ME coupling multiferroics is achieved. Our results not only reveal a design methodology to attain coexistence of ferroelectric and ferromagnetic orders in 2D materials but also provide insights into magnetoelectricity in 2D materials.