Realizing Room-Temperature Ferromagnetism in Molecular-Intercalated Antiferromagnet VOCl.

2D van der Waals (vdW) magnets are gaining attention in fundamental physics and advanced spintronics, due to their unique dimension-dependent magnetism and potential for ultra-compact integration. However, achieving intrinsic ferromagnetism with high Curie temperature (T C ) remains a technical challenge, including preparation and stability issues. Herein, an applicable electrochemical intercalation strategy to decouple interlayer interaction and guide charge doping in antiferromagnet VOCl, thereby inducing robust room-temperature ferromagnetism, is developed. The expanded vdW gap isolates the neighboring layers and shrinks the distance between the V-V bond, favoring the generation of ferromagnetic (FM) coupling with perpendicular magnetic anisotropy. Element-specific X-ray magnetic circular dichroism (XMCD) directly proves the source of the ferromagnetism. Detailed experimental results and density functional theory (DFT) calculations indicate that the charge doping enhances the FM interaction by promoting the orbital hybridization between t 2 g and e g . This work sheds new light on a promising way to achieve room-temperature ferromagnetism in antiferromagnets, thus addressing the critical materials demand for designing spintronic devices.