Using first-principles calculations, we investigate the magnetic order in two-dimensional (2D) transition-metal-dichalcogenide (TMD) monolayers: MoS₂, MoSe₂, MoTe₂, WSe₂, and WS₂ substitutionally doped with period four transition-metals (Ti, V, Cr, Mn, Fe, Co, Ni). We uncover five distinct magnetically ordered states among the 35 distinct TMD-dopant pairs: the non-magnetic (NM), the ferromagnetic with out-of-plane spin polarization (Z FM), the out-of-plane polarized clustered FMs (clustered Z FM), the in-plane polarized FMs (X–Y FM), and the anti-ferromagnetic (AFM) state. Ni and Ti dopants result in an NM state for all considered TMDs, while Cr dopants result in an anti-ferromagnetically ordered state for all the TMDs. Most remarkably, we find that Fe, Mn, Co, and V result in an FM ordered state for all the TMDs, except for MoTe₂. Finally, we show that V-doped MoSe₂ and WSe₂, and Mn-doped MoS₂, are the most suitable candidates for realizing a room-temperature FM at a 16–18% atomic substitution.

使用第一性原理计算，我们研究了二维（2D）过渡金属-二硫化碳（TMD）单层的磁阶：MoS ₂，MoSe ₂，MoTe ₂，WSe ₂和WS ₂周期地掺杂了四种过渡金属（Ti，V，Cr，Mn，Fe，Co，Ni）。我们揭示了35个不同的TMD掺杂剂对中的五个不同的磁有序状态：非磁性（NM），具有平面外自旋极化（Z FM）的铁磁，平面外极化群集FM（聚簇） Z FM），面内极化FM（X–Y FM）和反铁磁（AFM）状态。对于所有考虑的TMD，Ni和Ti掺杂剂会导致NM状态，而对于所有TMD，Cr掺杂剂会导致反铁磁有序状态。最值得注意的是，我们发现，除MoTe ₂之外，所有TMD的Fe，Mn，Co和V均呈FM有序状态。最后，我们显示了V掺杂的MoSe ₂和WSe ₂以及Mn掺杂的MoS ₂，是实现16-18％原子取代的室温FM的最合适的候选物。