Chiral superconductors, a unique class of unconventional superconductors in which the complex superconducting order parameter winds clockwise or anticlockwise in the momentum space¹, represent a topologically non-trivial system with intrinsic time-reversal symmetry breaking (TRSB) and direct implications for topological quantum computing^2,3. Intrinsic chiral superconductors are extremely rare, with only a few arguable examples, including UTe₂, UPt₃ and Sr₂RuO₄ (refs. ^4,5,6,7). It has been suggested that chiral superconductivity may exist in non-centrosymmetric superconductors^8,9, although such non-centrosymmetry is uncommon in typical solid-state superconductors. Alternatively, chiral molecules with neither mirror nor inversion symmetry have been widely investigated. We suggest that an incorporation of chiral molecules into conventional superconductor lattices could introduce non-centrosymmetry and help realize chiral superconductivity¹⁰. Here we explore unconventional superconductivity in chiral molecule intercalated TaS₂ hybrid superlattices. Our studies reveal an exceptionally large in-plane upper critical field B_c2,|| well beyond the Pauli paramagnetic limit, a robust π-phase shift in Little–Parks measurements and a field-free superconducting diode effect (SDE). These experimental signatures of unconventional superconductivity suggest that the intriguing interplay between crystalline atomic layers and the self-assembled chiral molecular layers may lead to exotic topological materials. Our study highlights that the hybrid superlattices could lay a versatile path to artificial quantum materials by combining a vast library of layered crystals of rich physical properties with the nearly infinite variations of molecules of designable structural motifs and functional groups¹¹.

手性超导体是一类独特的非常规超导体，其中复杂的超导有序参数在动量空间¹中顺时针或逆时针缠绕，代表了一种具有内在时间反转对称性破缺（TRSB）的拓扑非平凡系统，对拓扑量子计算有直接影响^2,3 .本征手性超导体极其罕见，只有几个有争议的例子，包括UTe ₂ 、UPt ₃和Sr ₂ RuO ₄ （参考文献^{4、5、6、7} ）。有人提出，手性超导性可能存在于非中心对称超导体中^8,9 ，尽管这种非中心对称性在典型的固态超导体中并不常见。或者，既不具有镜像对称性也不具有反演对称性的手性分子已被广泛研究。我们建议将手性分子纳入传统的超导晶格可以引入非中心对称性并有助于实现手性超导¹⁰ 。在这里，我们探索了手性分子插层 TaS ₂杂化超晶格中的非常规超导性。我们的研究揭示了异常大的面内上临界场B _c2,||远远超出泡利顺磁极限，Little-Parks 测量中具有强大的 π 相移以及无场超导二极管效应 (SDE)。这些非常规超导的实验特征表明，晶体原子层和自组装手性分子层之间有趣的相互作用可能会产生奇异的拓扑材料。 我们的研究强调，混合超晶格可以通过将具有丰富物理特性的庞大层状晶体库与可设计结构图案和官能团的分子的近乎无限变化相结合，为人造量子材料奠定一条通用的道路¹¹ 。