biostudies-literatureUnknown9(10)Qian ZDesign of two-dimensional (2D) multiferroic materials with two or more ferroic orders in one structure is highly desired in view of the development of next-generation electronic devices. Unfortunately, experimental or theoretical discovery of 2D intrinsic multiferroic materials is rare. Using first-principles calculation methods, we report the realization of multiferroics that couple ferromagnetism and ferroelectricity by intercalating Cu atoms in bilayer CrI₃, Cu_<i>x</i>@bi-CrI₃ (<i>x</i> = 0.03, 0.06, and 0.25). Our results show that the intercalation of Cu atoms leads to the inversion symmetry breaking of bilayer CrI₃ and produces intercalation density-dependent out-of-plane electric polarization, around 18.84-90.31 pC·cm^-2. Moreover, the switch barriers of Cu_<i>x</i>@bi-CrI₃ in both polarization states are small, ranging from 0.31 to 0.69 eV. Furthermore, the magnetoelectric coupling properties of Cu_<i>x</i>@bi-CrI₃ can be modulated via varying the metal ion intercalation density, and half-metal to semiconductor transition can be occurred by decreasing the intercalation density of metal ions. Our work paves a practical path for 2D magnetoelectron coupling devices.ACS omega11478-11483https://www.ebi.ac.uk/biostudies/studies/S-EPMC10938309biostudies-literatureCoexistence of Ferromagnetism and Ferroelectricity in Cu-Intercalated Bilayer CrI₃.PMC10938309Guo NQian ZRui XLu JGu GPeng QHua BWang YWang ZZhu TfalseCoexistence of Ferromagnetism and Ferroelectricity in Cu-Intercalated Bilayer CrI₃.Design of two-dimensional (2D) multiferroic materials with two or more ferroic orders in one structure is highly desired in view of the development of next-generation electronic devices. Unfortunately, experimental or theoretical discovery of 2D intrinsic multiferroic materials is rare. Using first-principles calculation methods, we report the realization of multiferroics that couple ferromagnetism and ferroelectricity by intercalating Cu atoms in bilayer CrI₃, Cu_<i>x</i>@bi-CrI₃ (<i>x</i> = 0.03, 0.06, and 0.25). Our results show that the intercalation of Cu atoms leads to the inversion symmetry breaking of bilayer CrI₃ and produces intercalation density-dependent out-of-plane electric polarization, around 18.84-90.31 pC·cm^-2. Moreover, the switch barriers of Cu_<i>x</i>@bi-CrI₃ in both polarization states are small, ranging from 0.31 to 0.69 eV. Furthermore, the magnetoelectric coupling properties of Cu_<i>x</i>@bi-CrI₃ can be modulated via varying the metal ion intercalation density, and half-metal to semiconductor transition can be occurred by decreasing the intercalation density of metal ions. Our work paves a practical path for 2D magnetoelectron coupling devices.2024-01-01T00:00:00Z2024 Mar2025-04-22T12:59:13.526Z2025-04-06T00:26:19.935ZS-EPMC109383093849695810.1021/acsomega.3c08360