Two-Dimensionality and Electron Doping Enhance Superconductivity in a SnSe2–Co(Cp)2 Organic–Inorganic Hybrid Superlattice

The tunability of transition metal dichalcogenides (TMDs) makes them ideal platforms for exploring emergent phenomena. While superconductivity has been observed in 1T-SnSe2 intercalated with cobaltocene Co(Cp)2, the underlying electronic mechanisms remain unclear. Using angle-resolved photoemission spectroscopy (ARPES), we investigate the electronic structure evolution from pristine 1T-SnSe2 to the SnSe2–Co(Cp)2 superlattice. We observe increased two-dimensionality in the superlattice and electron doping of the SnSe2 conduction band minimum. This dimensional change, combined with the higher charge carrier density, significantly increases the density of states near the Fermi level, a key factor for superconductivity. Our findings demonstrate the effectiveness of organic molecular intercalation for manipulating electronic dimensionality and inducing superconductivity in TMD-based heterostructures.