Intrinsic Magnetism and Field‐Driven Spin Alignment in NiI 2 Revealed by X‐ray Magnetic Spectroscopy

This study investigates the intrinsic magnetism and field‐driven spin alignment in NiI2 using X‐ray absorption spectroscopy and X‐ray magnetic circular dichroism (XMCD). NiI2, a van der Waals material, exhibits helimagnetic and type‐II multiferroic behavior. This study reveals robust XMCD signals across paramagnetic, antiferromagnetic, and helimagnetic phases under applied out‐of‐plane fields up to 6 T, while no net moment emerges at zero field. Atomic multiplet calculations confirm a covalent Ni 3d ground state with a significantly reduced spin moment. The results establish the intrinsic nature of NiI2's magnetism and clarify its field‐driven spin alignment mechanism. This comprehensive spectroscopic characterization lays the foundation for future applications of NiI2 in advanced spintronic and multiferroic devices, despite challenges posed by its low transition temperature in the monolayer limit. Future research should focus on enhancing its critical temperature through doping, strain engineering, or heterostructure fabrication.