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.