Imprinting Ferromagnetism and Superconductivity in Single Atomic Layers of Molecular Superlattices

Abstract Ferromagnetism and superconductivity are two antagonistic phenomena since ferromagnetic exchange fields tend to destroy singlet Cooper pairs. Reconciliation of these two competing phases has been achieved in vertically stacked heterostructures where these two orders are confined in different layers. However, controllable integration of these two phases in one atomic layer is a longstanding challenge. Here, an interlayer‐space‐confined chemical design (ICCD) is reported for the synthesis of dilute single‐atom‐doped TaS₂ molecular superlattice, whereby ferromagnetism is observed in the superconducting TaS₂ layers. The intercalation of 2H‐TaS₂ crystal with bulky organic ammonium molecule expands its van der Waals gap for single‐atom doping via co‐intercalated cobalt ions, resulting in the formation of quasi‐monolayer Co‐doped TaS₂ superlattices. Isolated Co atoms are decorated in the basal plane of the TaS₂ via substituting the Ta atom or anchoring at a hollow site, wherein the orbital‐selected p–d hybridization between Co and neighboring Ta and S atoms induces local magnetic moments with strong ferromagnetic coupling. This ICCD approach can be applied to various metal ions, enabling the synthesis of a series of crystal‐size TaS₂ molecular superlattices.