Magnetic skyrmions are potential candidates for high-density storage and logic devices because of their inherent topological stability and nanoscale size. Two-dimensional (2D) Janus transition metal chalcogenides (TMDs) are widely used to induce skyrmions due to the breaking of inversion symmetry. However, the experimental synthesis of Janus TMDs is rare, which indicates that the Janus configuration might not be the most stable MXY structure. Here, through machine-learning-assisted high-throughput first-principles calculations, we demonstrate that not all MXY compounds can be stabilized in Janus layered structure and a large proportion prefer to form other configurations with lower energy than the Janus configuration. Interestingly, these new configurations exhibit a strong Dzyaloshinskii–Moriya interaction (DMI), which can generate and stabilize skyrmions even under a strong magnetic field. This work provides not only an efficient method for obtaining ferromagnetic materials with strong DMI but also a theoretical guidance for the synthesis of TMDs via experiments.

磁性斯格明子因其固有的拓扑稳定性和纳米级尺寸而成为高密度存储和逻辑器件的潜在候选者。二维 （2D） Janus 过渡金属硫属化物 （TMD） 由于反转对称性的破坏而被广泛用于诱导斯格明子。然而，Janus TMD 的实验合成很少见，这表明 Janus 构型可能不是最稳定的 MXY 结构。在这里，通过机器学习辅助的高通量第一性原理计算，我们证明了并非所有 MXY 化合物都可以在 Janus 层状结构中稳定，并且很大一部分化合物更喜欢形成比 Janus 配置能量更低的其他构型。有趣的是，这些新构型表现出很强的 Dzyaloshinskii-Moriya 相互作用 （DMI），即使在强磁场下也能产生并稳定斯格明子。这项工作不仅为获得具有强 DMI 的铁磁材料提供了一种有效的方法，而且为通过实验合成 TMD 提供了理论指导。