Monolayer puckered pentagonal VTe2: An emergent two-dimensional ferromagnetic semiconductor with multiferroic coupling

Two-dimensional (2D) magnetic crystals have been extensively explored thanks to their potential applications in spintronics, valleytronics, and topological superconductivity. Here we report a novel monolayer magnet, namely puckered pentagonal VTe2 (PP-VTe2), intriguing atomic and electronic structures of which were firmly validated from first-principles calculations. The PP-VTe2 exhibits strong intrinsic ferromagnetism and semiconducting property distinct from the half-metallic bulk pyrite VTe2 (BP-VTe2) phase. An unusual magnetic anisotropy with large magnetic exchange energies is found. More interestingly, the multiferroic coupling between its 2D ferroelasticity and in-plane magnetization is further identified in PP-VTe2, lending it unprecedented controllability with external strains and electric fields. Serving as an emergent 2D ferromagnetic semiconductor with a novel crystal structure, monolayer PP-VTe2 provides an ideal platform for exploring exotic crystalline and spin configurations in low-dimensional systems.