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Abstract 2D magnetic semiconductors exhibit great potential for next‐generation spintronics, but realizing their full capabilities has been hindered by the low Curie temperatures ( T c ) below 50 K observed in current materials. Here, a new mechanism to substantially enhance the T c of 2D semiconducting materials through incorporating both in‐plane and out‐of‐plane superexchange interactions enabled by structural design is demonstrated. Specifically, monolayer Cr 2 Se 3 is synthesized with a five‐layer Se–Cr–Se–Cr–Se atomic structure using molecular beam epitaxy (MBE). This unique structure not only possesses optimized in‐plane superexchange interaction but also incorporates out‐of‐plane Cr–Se–Cr couplings. Scanning tunneling spectroscopy (STS) and angular‐resolved photoemission spectroscopy (ARPES) confirm its semiconducting nature. Remarkably, the ferromagnetic phase transition observed by ARPES and Magnetic Force Microscopy (MFM) indicated that its T c is up to 230 K. This not only establishes a new record for T c in 2D ferromagnetic semiconductor materials but also introduces a novel approach to modulating materials' properties by manipulating the vertical dimension in 2D materials.
Lu et al. (Wed,) studied this question.