Breaking the Trade-off: Bulk 2D Ising Superconductivity with High Tc and Giant Interlayer Spacing via a Unique Chain Intercalation in (BaS)1/3TaS2.

Two-dimensional (2D) transition-metal dichalcogenides (TMDs) are promising platforms for low-dimensional superconductivity. However, in conventional intercalated systems, achieving a high superconducting transition temperature (Tc) often comes at the expense of reduced interlayer spacing and weakened 2D character. Here, we overcome this long-standing compromise through a unique chain-like intercalation strategy. We report the synthesis and properties of a new polymorph, (BaS)1/3TaS2, in which a distinctive Ba-S-S-Ba chain structure is inserted between TaS2 bilayers. This unique configuration breaks the bulk c-axis mirror symmetry while achieving exceptional interlayer decoupling, with an interbilayer spacing of 12.75 Å─more than three times that of pristine 2H-TaS2. By suppressing interlayer electronic coupling, this structural evolution allows local inversion symmetry breaking within individual TaS2 layers to dominate. This prevents compensation of the Ising spin-orbit fields typical of centrosymmetric bulk phases, enabling robust 2D Ising superconductivity. Remarkably, the compound exhibits an enhanced Tc without sacrificing its large interlayer spacing, thereby breaking the conventional trade-off between "large spacing/high anisotropy" and "high Tc". Comprehensive transport, magnetic, and thermodynamic measurements confirm its robust superconducting state. Our work establishes a versatile intercalation framework for designing bulk-like 2D Ising superconductors, providing a new route to reconcile competing material demands and expanding the scope of Ising superconductivity research.