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. [Figure not available: see fulltext.].