Giant piezoelectricity in antiferromagnetic CrS2 and CrSe2 monolayers

Abstract Two-dimensional (2D) materials, particularly transition metal dichalcogenides (TMDs), have garnered significant attention in the nanoscale piezoelectric field due to their high crystallinity and ability to withstand large strains. Through density-functional theory calculations, we have discovered that monolayer H-phase CrS 2 and CrSe 2 exhibit antiferromagnetic semiconducting properties, in contrast to the previously held belief that they were nonmagnetic (NM) semiconductors. While the piezoelectric coefficients of NM CrS 2 and CrSe 2 are comparable to those of MoS 2 , their antiferromagnetic ground states demonstrate significantly enhanced piezoelectric coefficients ( d 11 ) of 27.66 pm V −1 and 52.36 pm V −1 , respectively. These values exceed that of MoS 2 by an order of magnitude, marking the highest recorded for TMD materials and the highest in 2D magnetic materials to date. The greatly enhanced piezoelectric responses in the antiferromagnetic states of CrS 2 and CrSe 2 compared to their NM states arise from three primary factors. Firstly, the displacement of the Wannier center under strain is more pronounced in the antiferromagnetic state, leading to a greater change in dipole moment (enhanced clamped-ion contribution). Secondly, there is a heightened polarization change due to internal atomic distortions (internal-strain term) in response to macroscopic strain in the antiferromagnetic state. Thirdly, the material undergoes a softening of the elastic coefficient in its antiferromagnetic state. These findings open new avenues for designing high-performance piezoelectric and magnetic multifunctional materials.