First-principles study of the electronic structure, magnetism and optical properties of 5d-metal-doped PtSe 2 /ZrS 2 heterostructures

Abstract This study systematically investigates the regulatory effects of 5d transition metal doping (Ta, W, Re, and Os) on the electronic structure, magnetism, and optical properties of PtSe 2 /ZrS 2 van der Waals heterojunctions using density functional theory. Results indicate that the intrinsic PtSe 2 /ZrS 2 heterostructure exhibits nonmagnetic semiconductor behavior. However, introducing 5d metal doping effectively lifts the spin degeneracy, yielding diverse electronic and magnetic responses. Different doping elements and their occupancy patterns significantly influence the system’s band structure, enabling tunable transitions between semiconductor, metallic, and half-metal-like electronic characteristics. The Ta/W doping configuration and the Os doping configuration exhibit distinct and opposite spin-asymmetric electronic structure characteristics near the Fermi level. Magnetic analysis reveals that the doping-induced magnetic moment is primarily localized on the 5d-doped atoms, while the host atoms exhibit only weak induced spin polarization. Optical property studies further demonstrate that 5d doping and its site selection can significantly alter the absorption intensity, peak position, and low-energy reflection behavior of the heterojunction. These results demonstrate that rational design of 5d dopant elements and doping sites enables synergistic control over the electronic, magnetic, and optical properties of PtSe 2 /ZrS 2 heterojunctions, providing theoretical justification for their potential applications in spintronic and optoelectronic devices.