Abstract Graphene is a promising candidate for spintronics and low-dissipation quantum electronic device applications. However, its excessively weak spin-orbit coupling interaction (~ 24.0 μeV) makes the electric field modulation of spin currents almost impossible and the experimental observation of spin-polarized edge states in topological energy gap very challenging. These difficulties limit the practical applications of graphene. In this work, the electronic structures and topological properties of group IVB transition metal M-doped graphene (M = Ti, Zr, Hf) have been studied by first-principles calculations. Taking the Hf-doped graphene as an example, in the absence of spin-orbit coupling, this system possesses six equivalent Dirac points near the Fermi level in the Brillouin zone, owing to C 3z and inversion symmetries. These Dirac points exhibit linear dispersion in a wide energy range (about 1.00 eV), making this material a Dirac semimetal. When spin-orbit coupling interaction is considered, the Dirac points of this system are gapped with a spin-orbit gap of 16.4 meV, which is three orders of magnitude larger than that of graphene. Furthermore, the system is an intrinsic quantum spin Hall insulator with the nontrivial topological index Z 2 = 1. We also propose that the nontrivial topological properties are robust in a wide biaxial strain range from −5% to 5% and the spin-orbit gap further increases to 37.7 meV under 5% strain. Compared to the pristine graphene, our research has greatly enhanced spin-orbit coupling in this system with its nontrivial topological property preserved, which is crucial for the development of graphene-based spin field effect transistors. Moreover, such graphene-based robust topological material designs could also pave the way for a new generation of spintronics, ultra-low-dissipation electronics and quantum information processing devices.
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