Spin-Gapless States in Two-Dimensional Molecular Ferromagnet Fe2(TCNQ)2.

Abstract

Two-dimensional van der Waals magnetic atomic crystals have provided unprecedented access to magnetic ground states due to a quantum confinement effect. Here, using first-principles calculations, we demonstrate a spin-gapless molecular ferromagnet, namely, Fe2(TCNQ)2, with superior mechanical stability and a remarkable linear Dirac cone, which can be exfoliated from its already-synthesized van der Waals crystal. Especially, Young s modulus has values of 175.28 GPa·nm along the x- and y-directions with a Poisson s ratio of 0.29, while the Curie temperature within the Ising model is considerably higher than room temperature. Furthermore, spin-orbit coupling can open a band gap at the Dirac point, leading to topologically nontrivial electronic states characterized by an integer value of the Chern number and the edge states of its nanoribbon. Our results offer versatile platforms for achieving plastic spin filtering or a quantum anomalous Hall effect with promising applications in spintronics devices.