Modifying the Electronic and Magnetic Properties of ZrO2${\rm ZrO}_{2}$ Monolayer Through <i>Sp</i> Doping: A First‐Principles Study

Abstract Designing 2D materials for multifunctional applications becomes increasingly important because of the development of diminutive devices. In this work, doping with non‐transition metals (M@ systems; M = Na, Mg, Al, and Si) and nonmetals (X@ systems; X = B, C, N, and F) is proposed to modify the electronic and magnetic properties of monolayer. Pristine monolayer is a 2D insulator with a large bandgap of 4.40(6.08) eV obtained from standard(hybrid)‐based calculations. The monolayer is magnetized with total magnetic moments of 3.00, 2.00, and 1.00 upon doping with Na, Mg, and Al metals, respectively. In these cases, magnetic properties are produced mainly by O atoms around doping sites. Meanwhile, Si doping induces no magnetism in monolayer, preserving its nonmagnetic nature. However, the bandgap suffers from a large reduction of the order of 22.27%. The monolayer magnetization is also achieved by doping with B, C, N, and F atoms, where total magnetic moments of 3.00, 2.00, 1.00, and 0.97 are obtained, respectively. For ‐type doping cases, nonmetal impurities produce mainly magnetic properties, meanwhile, Zr atoms generate mainly the magnetism of F‐doped monolayer. Interestingly, feature‐rich half‐metallic nature (in Na@, Mg@, C@, and F@ systems) and magnetic semiconductor nature (in Al@, B@, and N@ systems) are also obtained. By analyzing Bader charge, the roles of charge loser and charge gainer are confirmed for non‐transition metal and nonmetal impurities, respectively. The results may introduce new 2D materials suitable for spintronic applications.