Tunable electronic structure and magnetic coupling in strained two-dimensional semiconductor MnPSe3

The electronic structures and magnetic properties of strained monolayer MnPSe3 are investigated systematically via first-principles calculations. It is found that the magnetic ground state of monolayer MnPSe3 can be significantly affected by biaxial strain engineering, while the semiconducting characteristics are well-preserved. Owing to the sensitivity of the magnetic coupling towards structural deformation, a biaxial tensile strain of approximately 13% can lead to an antiferromagnetic (AFM)- ferromagnetic (FM) transition. The strain-dependent magnetic stability is mainly attributed to the competition of the direct AFM interaction and indirect FM superexchange interaction between the two nearest-neighbor Mn atoms. In addition, we find that FM MnPSe3 is an intrinsic half semiconductor with large spin exchange splitting in the conduction bands, which is crucial for the spin-polarized carrier injection and detection. The sensitive interdependence among the external stimuli, electronic structure, and magnetic coupling makes monolayer MnPSe3 a promising candidate for spintronics.