Direct synthesis of controllable ultrathin heteroatoms-intercalated 2D layered materials

Two-dimensional (2D) layered materials have been studied in depth during the past two decades due to their unique structure and properties. Transition metal (TM) intercalation of layered materials have been proven as an effective way to introduce new physical properties, such as tunable 2D magnetism, but the direct growth of atomically thin heteroatoms-intercalated layered materials remains untapped. Herein, we directly synthesize various ultrathin heteroatoms-intercalated 2D layered materials (UHI-2DMs) through flux-assisted growth (FAG) approach. Eight UHI-2DMs (V_1/3NbS₂, Cr_1/3NbS₂, Mn_1/3NbS₂, Fe_1/3NbS₂, Co_1/3NbS₂, Co_1/3NbSe₂, Fe_1/3TaS₂, Fe_1/4TaS₂) were successfully synthesized. Their thickness can be reduced to the thinnest limit (bilayer 2D material with monolayer intercalated TM), and magnetic ordering can be induced in the synthesized structures. Interestingly, due to the possible anisotropy-stabilized long-range ferromagnetism in Fe_1/3TaS₂ with weak interlayer coupling, the layer-independent magnetic ordering temperature of Fe_1/3TaS₂ was revealed by magneto-transport properties. This work establishes a general method for direct synthesis of heteroatom-intercalated ultrathin 2D materials with tunable chemical and physical properties.