Great efforts have been taken towards in-plane structural extension of two-dimensional materials. Compared with surface lattices, edge lattices represent non-equilibrium states and remain largely unexplored. Herein, we report the all-physical top-down production of sub-1 nm molybdenum disulfide (MoS₂) and tungsten disulfide (WS₂) with 100% broken lattice. Bulk MoS₂ and WS₂ are tailored into subnanometer species with satisfactory yields (7.2 and 4.8 wt%) by sequential combination of dual and triple synergy silica-assisted ball-milling. Such two-stage ball-milling push the top-down limit into single-lattice scale, which is far beyond the manufacturing capacity of any known top-down method. Exceptional solvent diversity and solvability of the sub-1 nm MoS₂ and WS₂ powder endow solution-processability towards hybrid thin film fabrication. The sub-1 nm intrinsic MoS₂ and WS₂ demonstrate comprehensively superior performances over those of their bulk, nanosheets, and quantum sheets. Both photoluminescence and nonlinear saturation absorption of sub-1 nm MoS₂ and WS₂ are extremely enhanced. The non-equilibrium states induced by the entirely exposed and broken, intrinsic lattices in sub-1 nm MoS₂ and WS₂ could be determinative to their extreme performances. Our work highlights the potential of broken lattice and opens up an avenue towards subnanometer materials.

人们在二维材料的面内结构延伸方面付出了巨大的努力。与表面晶格相比，边缘晶格代表非平衡态，并且在很大程度上仍未被探索。_{在此，我们报告了100％晶格破碎的亚1纳米二硫化钼（MoS 2} ）和二硫化钨（WS _{2 ）}的全物理自上而下生产。通过连续组合双重和三重协同二氧化硅辅助球磨，将块状 MoS ₂和 WS _{2定制为亚纳米物质，产率令人满意（7.2 和 4.8 wt%）。}这种两级球磨将自上而下的极限推向单晶格规模，这远远超出了任何已知自上而下方法的制造能力。亚 1 nm MoS ₂和 WS ₂粉末具有出色的溶剂多样性和可溶性，赋予混合薄膜制造的溶液加工性能。亚1纳米本征MoS ₂和WS ₂表现出比块体、纳米片和量子片更优越的性能。亚1 nm MoS ₂和WS ₂的光致发光和非线性饱和吸收都极大增强。_{亚 1 nm MoS 2}和 WS ₂中完全暴露和破碎的本征晶格引起的非平衡态可能决定其极端性能。我们的工作强调了破碎晶格的潜力，并为亚纳米材料开辟了一条途径。