Probing the Néel-Type Antiferromagnetic Order and Coherent Magnon–Exciton Coupling in Van Der Waals VPS₃

2D van der Waals (vdW) antiferromagnets have received intensive attention due to their terahertz resonance, multilevel magnetic-order states, and ultrafast spin dynamics. However, accurately identifying their magnetic configuration still remains a challenge owing to the lack of net magnetization and insensitivity to external fields. In this work, the Néel-type antiferromagnetic (AFM) order in 2D antiferromagnet VPS₃ with the out-of-plane anisotropy, which is demonstrated by the temperature-dependent spin–phonon coupling and second-harmonic generation (SHG), is experimentally probed. This long-range AFM order even persists at the ultrathin limit. Furthermore, strong interlayer exciton–magnon coupling (EMC) upon the Néel-type AFM order is detected based on the monolayer WSe₂/VPS₃ heterostructure, which induces an enhanced excitonic state and further certifies the Néel-type AFM order of VPS₃. The discovery provides optical routes as the novel platform to study 2D antiferromagnets and promotes their potential applications in magneto-optics and opto-spintronic devices.