Computational design of the novel Fe-doped single-layer SrS: structural, electro-magnetic, and optical properties.

The search for novel intrinsic two-dimensional (2D) magnetic materials is crucial to understand the fundamentals of 2D magnetism and realize next-generation magneto-electric and magneto-optical systems. Using the rigorous framework of spin-polarized density functional theory (SPDFT)-based ab initio calculations, this investigation systematically investigates the effects of a stepwise change in the Fe composition ( x ) on the structural, electro-magnetic and optical properties of the ordered SrS based single-layer alloys, with x encompassing values from 0 to 1. Our comprehensive analysis revealed that the calculated formation energies, cohesive energies, phonon dispersions, molecular dynamics, and elastic constants of both bare SrS and FeS monolayers indicate their thermodynamic, dynamic, thermal, and mechanical stability in hexagonal and square structures, respectively. Significantly, the introduction of magnetic Fe dopants into the non-magnetic SrS semiconductor enabled the creation of an intrinsic magnetic (FM) state characterized by spin-polarized charge carriers at the Fermi level ( E F ). As doping increases, the electronic structure shows a noticeable dependence on the chemical composition. It is noteworthy that the systems doped with 0.750 and 1 Fe exhibit metallic-magnetic and metallic non-magnetic properties, respectively, and the rest are half-semiconductors (HSC) according to the GGA approximation. Conversely, the HSE approach shows a transition to HSC for a doping level of 0.750, while others maintain the same behavior. The study of the optical properties shows improvements compared to the bare SrS monolayer through the incorporation of Fe dopants. The bare SrS has light absorption in the ultraviolet region, while the absorption band edges for HSC compounds change from the infrared to visible regions. This study proposes a practical method to tune the properties of the SrS single-layer by selectively adjusting the dopant concentration. Such control is promising for applications in spintronics and optical based nanodevices.