Abstract

Despite growing interest in them, highly crystalline two-dimensional superconductors derived from exfoliated layered materials are few. Employing the anisotropic Migdal-Eliashberg formalism based on {\it ab initio} calculations, we find monolayer NiTe2_{2} to be an intrinsic superconductor with a Tc∼T_{\text c}\sim5.7~K, although the bulk crystal is not known to superconduct. Remarkably, bilayer NiTe2_{2} intercalated with lithium is found to display two-gap superconductivity with a critical temperature Tc∼11.3T_{\text{c}}\sim 11.3~K and superconducting gap of ∼\sim3.1~meV, arising from a synergy of electronic and phononic effects. The comparatively high TcT_\text{c}, substrate independence and proximity tunability will make these superconductors ideal platforms for exploring intriguing correlation effects and quantum criticality associated two-dimensional superconductivity.

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