Interlayer‐Incorporation of MoS₂ (TM‐MoS₂) to Achieve Unique Magnetic and Electronic Properties for Spintronics

Abstract The multi‐layer 2D materials have attracted increasing interest because the intriguing properties can be achieved by various strategies, such as incorporating ions into the interlayer, turning angles between two layers, and applying strain, which may lead to wide applications in catalysis, ion‐batteries, superconductors, and nanodevices. In this work, there is a proposal to tune the electronic and magnetic properties of MoS₂ bilayer for spintronics by incorporating transition‐metal elements into its interlayer (denoted as TM‐MoS₂) based on the density‐functional theory (DFT) calculations. It is shown that TM‐MoS₂ is thermodynamically stable and can be achieved due to low incorporation energy. It is found that n‐type doping or intrinsic semiconducting can be realized in MoS₂ bilayer by controlling the incorporated transition‐metal atoms, accompanied with a rich variety of magnetic orderings. It is further shown that the electronic and magnetic properties of TM‐MoS₂ can be substantially tuned by applying compression. Finally, it is demonstrated that the systems can be used as a spin filter, as supported by the spin‐polarized transport calculation. The findings illustrate that the physical properties of layered materials can be controlled by simple interlayer incorporation and shed light on the application of TM‐MoS₂ as a fundamental building block for nanoelectronics and spintronics.