In chiral materials, spins and chirality are coupled via spin-orbit interaction, provoking a fast-growing field of chiral spintronics. Compared with the widely explored chiral molecules, exploration of chirality-dependent spin effects in crystals and supramolecules remain limited. Here we assemble chiral superatomic crystals MXTe₄ (M = transition metal; X = Ga or Ge) using telluride tetrahedra clusters as building blocks. Distinct from atomic crystals, these assembled monolayers have tunable symmetries and electronic characteristics by tilting the tetrahedral units through the variation of inter-cluster interaction. Dresselhaus-type spin textures and anisotropic spin Hall effect with inversed sign of spin current under opposite geometrical handedness are demonstrated in these chiral monolayers by symmetry analysis and verified by ab initio calculations. These results provide an innovative paradigm for assembling superatomic crystals with designated symmetry and hierarchical structures to access the chirality-driven quantum effects.

在手性材料中，自旋和手性通过自旋轨道相互作用耦合，引发了手性自旋电子学领域的快速发展。与广泛探索的手性分子相比，晶体和超分子中手性依赖性自旋效应的探索仍然有限。在这里，我们使用碲化物四面体簇作为构建块组装手性超原子晶体 MXTe ₄（M = 过渡金属；X = Ga 或 Ge）。与原子晶体不同，这些组装的单分子层通过簇间相互作用的变化来倾斜四面体单元，从而具有可调的对称性和电子特性。通过对称分析，在这些手性单分子层中证明了德雷塞尔豪斯型自旋织构和在相反几何旋向下具有相反的自旋电流符号的各向异性自旋霍尔效应，并通过从头计算验证。这些结果为组装具有指定对称性和分层结构的超原子晶体提供了一种创新范例，以实现手性驱动的量子效应。