Two-dimensional anion-rich NaCl<sub>2</sub> crystal under ambient conditions.

Yi, Ruobing; Jiang, Jie; Yang, Yizhou; Zhang, Yueyu; Gao, Siyan; Zhao, Yimin; Hu, Jiahao; Su, Xuchang et al. · Nat Commun · 2025

basic_science · Level V

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Abstract

The two-dimensional (2D) "sandwich" structure composed of a cation plane located between two anion planes, such as anion-rich CrI<sub>3</sub>, VS<sub>2</sub>, VSe<sub>2</sub>, and MnSe<sub>2</sub>, possesses exotic magnetic and electronic structural properties and is expected to be a typical base for next-generation microelectronic, magnetic, and spintronic devices. However, only a few 2D anion-rich "sandwich" materials have been experimentally discovered and fabricated, as they are vastly limited by their conventional stoichiometric ratios and structural stability under ambient conditions. Here, we report a 2D anion-rich NaCl<sub>2</sub> crystal with sandwiched structure confined within graphene oxide membranes with positive surface potential. This 2D crystal has an unconventional stoichiometry, with Na:Cl ratio of approximately 1:2, resulting in a molybdenite-2H-like structure with cations positioned in the middle and anions in the outer layer. The 2D NaCl<sub>2</sub> crystals exhibit room-temperature ferromagnetism with clear hysteresis loops and transition temperature above 320 K. Theoretical calculations and X-ray magnetic circular dichroism (XMCD) spectra reveal the ferromagnetism originating from the spin polarization of electrons in the Cl elements of these crystals. Our research presents a simple and general approach to fabricating advanced 2D unconventional stoichiometric materials that exhibit half-metal and ferromagnetism for applications in electronics, magnetism, and spintronics.