Spin-Orbit Coupling and Spin-Polarized Electronic Structures of Janus Vanadium-Dichalcogenide Monolayers: First-Principles Calculations

Abstract

Phonon and spintronic structures of monolayered Janus vanadium-dichalcogenide compounds are calculated by the first-principles schemes of pseudopotential plane-wave based on spin-density functional theory, to study dynamic structural stability and electronic spin-splitting due to spin-orbit coupling (SOC) and spin polarization. Geometry optimizations and phonon-dispersion spectra demonstrate that vanadium-dichalcogenide monolayers possess a high enough cohesive energy, while VSTe and VTe2 monolayers specially possess a relatively higher in-plane elastic coefficient and represent a dynamically stable structure without any virtual frequency of atomic vibration modes. Atomic population charges and electron density differences demonstrate that V–Te covalent bonds cause a high electrostatic potential gradient perpendicular to layer-plane internal VSTe and VSeTe monolayers. The spin polarization of vanadium 3d-orbital component causes a pronounced energetic spin-splitting of electronic-states near the Fermi level, leading to a semimetal band-structure and increasing optoelectronic band-gap. Rashba spin-splitting around G point in Brillouin zone can be specifically introduced into Janus VSeTe monolayer by strong chalcogen SOC together with a high intrinsic electric field (potential gradient) perpendicular to layer-plane. The vertical splitting of band-edge at K point can be enhanced by a stronger SOC of the chalcogen elements with larger atom numbers for constituting Janus V-dichalcogenide monolayers. The collinear spin-polarization causes the band-edge spin-splitting across Fermi level and leads to a ferrimagnetic order in layer-plane between V and chalcogen cations with higher α and β spin densities, respectively, which accounts for a large net spin as manifested more apparently in VSeTe monolayer. In a conclusion for Janus vanadium-dichalcogenide monolayers, the significant Rashba splitting with an enhanced K-point vertical splitting can be effectively introduced by a strong SOC in VSeTe monolayer, which simultaneously represents the largest net spin of 1.64 (ћ/2) per unit cell. The present study provides a normative scheme for first-principles electronic structure calculations of spintronic low-dimensional materials, and suggests a prospective extension of two-dimensional compound materials applied to spintronics.