Two-dimensional (2D) atomic crystal superlattices integrate diverse 2D layered materials enabling adjustable electronic and optical properties. However, tunability of the interlayer gap and interactions remain challenging. Here we report a solution based on soft oxygen plasma intercalation. 2D atomic crystal molecular superlattices (ACMSs) are produced by intercalating O₂⁺ ions into the interlayer space using the plasma electric field. Stable molecular oxygen layer is formed by van der Waals interactions with adjacent transition metal dichalcogenide (TMD) monolayers. The resulting interlayer gap expansion can effectively isolate TMD monolayers and impart exotic properties to homo-(MoS₂[O₂]_x) and hetero-(MoS₂[O₂]_x/WS₂[O₂]_x) stacked ACMSs beyond typical capacities of monolayer TMDs, such as 100 times stronger photoluminescence and 100 times higher photocurrent. Our potentially universal approach to tune interlayer stacking and interactions in 2D ACMSs may lead to exotic superlattice properties intrinsic to monolayer materials such as direct bandgap pursued for future optoelectronics.

二维（2D）原子晶体超晶格集成了多种2D分层材料，可实现可调的电子和光学特性。然而，层间间隙和相互作用的可调性仍然具有挑战性。在这里，我们报告基于软氧等离子体嵌入的解决方案。二维原子晶体分子超晶格（ACMS）是通过使用等离子电场将O ₂ ⁺离子插入层间空间而产生的。稳定的分子氧层是通过范德华斯与相邻的过渡金属二卤化硅（TMD）单层相互作用而形成的。产生的层间间隙扩展可以有效地隔离TMD单层，并赋予均质（MoS ₂ [O ₂ ] _x）和异质（MoS ₂[O ₂ ] _x / WS ₂ [O ₂ ] _x）堆叠的ACMS超出了单层TMD的典型容量，例如光致发光强度高100倍，光电流高100倍。我们在2D ACMS中调整层间堆叠和相互作用的潜在通用方法可能会导致单层材料固有的奇异超晶格特性，例如为未来的光电子学所追求的直接带隙。