Surface‐Sensitive Detection of Magnetic Phase Transition in Van Der Waals Magnet CrSBr.

2D magnets have recently drawn enormous interest. As an air‐stable A‐type van der Waals antiferromagnet (AFM), CrSBr has attracted great attention but has also led to controversies about its large‐span ordering temperatures. Herein, a systematic study of the magnetic phase transition in single‐crystalline CrSBr with ultrahigh‐quality through surface‐sensitive X‐ray magnetic linear dichroism and X‐ray magnetic circular dichroism measurements combined with vibrating sample magnetometry for characterization of bulk magnetization is reported. The interlayer AFM order of both surface and bulk CrSBr is revealed to maintain a similar Néel temperature within the range of 132–142 K. However, the intralayer ferromagnetic (FM) order of surface CrSBr is found to sustain up to ≈238 K, 70 K higher than the value obtained from the bulk CrSBr, demonstrating a dramatically different surface and bulk Curie temperature in CrSBr. Moreover, a half‐filled t2g electronic state for Cr3+ ions with magnetic moment of ≈3 µB/Cr in CrSBr is clearly identified. These results enrich the understanding of the electronic structure and magnetism in CrSBr, providing this material as a promising building block for future spintronic devices. [ABSTRACT FROM AUTHOR]