Strain-tunable magnetism in monolayer puckered pentagonal VTe2

The discovery of intrinsic two-dimensional (2D) magnetic materials has opened new avenues for exploring low-dimensional magnetism and spintronic functionalities. Among various control strategies, strain engineering provides a versatile and efficient approach for modulating the magnetic and electronic properties of 2D systems. In this work, we investigate a novel 2D puckered pentagonal phase VTe2 (PP-VTe2) and find that it hosts intrinsic bipolar magnetic semiconducting behavior with strong strain-dependent magnetic properties. The magnetization direction of PP-VTe2 can be regulated by applying strain, transforming the in-plane easy magnetization plane into an out-of-plane easy magnetization axis. The modulation of magnetic exchange interaction under strain is direction-dependent, and the Curie temperature (TC) shows adjustability and robustness under compressive strain and tensile strain, respectively. The tunable magnetism of PP-VTe2 under strain is explained microscopically by analyzing spin–orbit coupling and magnetic exchange interaction. In addition, the magneto-optical Kerr effect of PP-VTe2 was studied, which has good magneto-optical responsivity, which is conducive to its application in non-contact magneto-optical responsive devices. These findings demonstrate that structural distortion under strain influences spin ordering in PP-VTe2, unraveling mechanisms for 2D magnetism control and highlighting routes toward strain-engineered spintronics.