Elemental Substitution Alters Antiferromagnetic Order in CrPS₄

Layered magnetic semiconductors are of particular interest as they couple magnetic order with semiconducting functionality, enabling tunable low dimensional magnetism while offering practical pathways toward two dimensional (2D) spintronic devices. In this work, we demonstrate that elemental substitution constitutes a synthetic strategy to simultaneously tailor magnetic order and electronic structure in the layered antiferromagnetic semiconductor. We synthesize and systematically characterize a series of V-substituted CrPS₄ single crystals, Cr₁₋ₓVₓPS₄ (0 ≤ x ≤ 0.43), which retain the parent crystal structure CrPS₄ with V atoms randomly occupying Cr sites. Progressive V substitution induces a pronounced evolution of magnetic ground states, driving a transition from A-type to Néel-type antiferromagnetic order, accompanied by a continuous reduction of the electronic bandgap. These results establish elemental substitution as a broadly applicable route to tune the coupled spin and electronic degrees of freedom in layered antiferromagnetic semiconductors, also providing a versatile platform for further multifunctional device applications.