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
x
@bi-CrI3 (x = 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
x
@bi-CrI3 in both polarization states are small, ranging
from 0.31 to 0.69 eV. Furthermore, the magnetoelectric coupling properties
of Cu
x
@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.