Abstract

The existence of superconductivity (SC) appears to be established in both twisted and nontwisted graphene multilayers. However, whether their building block, single-layer graphene (SLG), can also host SC remains an open question. Earlier theoretical works predicted that SLG could become a chiral d-wave superconductor driven by electronic interactions when doped to its van Hove singularity, but questions such as whether the d-wave SC survives the strong band renormalizations seen in experiments, its robustness against the source of doping, or if it will occur at any reasonable critical temperature (Tc) have remained difficult to answer, in part due to uncertainties in model parameters. Furthermore, doping of graphene beyond its van Hove singularity remained experimentally challenging and was not demonstrated until recently. In this study, we n dope SLG past the van Hove singularity by employing Tb intercalation and derive structural models from angle-resolved photoemission spectroscopy measurements. We adopt a reliable numerical framework based on a random-phase approximation technique to investigate the emergence of unconventional SC in the heavily doped monolayer. We predict that robust d + id topological SC could arise in SLG doped by Tb, with a Tc up to 600 mK. We also employ first-principles calculations to investigate the possibility of realizing d-wave SC with other dopants, such as Li or Cs. We find that dopants that change the lattice symmetry of SLG are detrimental to the d-wave state. The stability of the d-wave SC predicted here in Tb-doped SLG could provide a valuable insight for guiding future experimental efforts aimed at exploring topological superconductivity in monolayer graphene.

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