Evolution of the Magnetic Ground States in Mn-Intercalated 2 H -TaS ₂ Crystals

Because of their rich and highly tunable physical properties, TaS₂-based crystals have become a prominent platform for condensed matter research. Most previous studies of 2H-MxTaS₂ have focused on intercalation concentrations of 1/4 and 1/3. However, some recent reports reveal that the nonstoichiometric compositions (deviating from the 1/4 and 1/3 ratios) could also exhibit novel physical properties. Here, the magnetic properties of 2H-MnxTaS₂ single crystals (0.089 ≤ x ≤ 0.472) are systematically investigated, where the Mn ions are intercalated into the vdW gaps of the 2H-TaS₂ phase. Mn intercalation induces distinct magnetic ground states: a cluster spin glass (CSG) state (x ≤ 0.206), an in-plane soft ferromagnetic (FM) state (0.206 ≤ x < 0.392) with the highest Curie temperature (TC ∼ 105 K) at x = 0.282, and an antiferromagnetic (AFM) state (x ≥ 0.392). The transition between the FM and AFM states, as well as the maximum TC, is attributed to the periodic oscillation of the 2D Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction caused by the variation of interlayer Mn spacing. These results provide new insights into the tunable magnetic ground states of transition-metal-intercalated 2H-TaS₂ systems.