Graphical Abstract
![](https://wqketang.oss-cn-beijing.aliyuncs.com/unzip/large-zip/zip-97503eea-e437-460b-aca5-621c9c7f10fb/6855/files/6855-TOC.jpg?Expires=1725757997&OSSAccessKeyId=STS.NSssK71aLjDMY9SbRgGRGskMT&Signature=QyJpHTDVPY%2BB5o1Bq9cMH4ZeGeM%3D&security-token=CAISywJ1q6Ft5B2yfSjIr5DGOPGD3L5t3YamWx%2FihlIyS91rnK7mtjz2IHtKenhsBOsbtfk1mG5W5%2FgZlqJ9SptIAEfJa9d99Myjb%2F9FltCT1fau5Jko1beHewHKeTOZsebWZ%2BLmNqC%2FHt6md1HDkAJq3LL%2Bbk%2FMdle5MJqP%2B%2FUFB5ZtKWveVzddA8pMLQZPsdITMWCrVcygKRn3mGHdfiEK00he8TouufTinpHMskGA1Aell7Mvyt6vcsT%2BXa5FJ4xiVtq55utye5fa3TRYgxowr%2Fwo0v0YpGya5YzHXwcPskvdKZbo78UqLQlla6w%2BGqFJqvPxr%2Fp8t%2Fx5fWJKAezhVgs8cVM8JOjIqKOscIsixo262SmqFV55c8Fdm%2BgUooJVgIMhTnduUfAPJAGOxzJitP%2BUVGGphr60TEnBL4rB5MUctfzRpwT64j3UTzDnGoABhFRSspTLrn9GrEN9pQYzC6eepGdfWDQh3fr5hA1VnwVUJMCz%2BNQEDWKceF%2FnEjWVMtfbvqYxuyhSCmIMMyh5bEREEKEiD%2BFVv4ZfsqnV7hQy5w6HhIkN8kZzP6L0zPvPgkBLOtdMDeDxhf8dVPrCSG4etXHjxcwUaRVb3ZR7Yu8gAA%3D%3D)
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Two-dimensional (2D) semiconductors with intrinsic ferromagnetism are highly desirable for potential applications in next-generation spintronic and optoelectronic devices. However, controllable synthesis of intrinsic 2D magnetic semiconductor on a substrate is still a challenging task. Herein, large-area 2D non-layered rock salt (α-phase) MnSe nanosheets were grown on mica substrates, with the thickness changing from 54.2 to 0.9 nm (one unit cell), by chemical vapour deposition. The X-ray diffraction, Raman spectroscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy measurements confirmed that the resulting 2D α-MnSe nanosheets were obtained as high-quality single crystals. The magnetic hysteresis loops and synchrotron X-ray measurements directly indicated the anomalous magnetic properties in α-MnSe nanosheets. Comprehensive analysis of the reasons for magnetic property revealed that the low-temperature phase transition, small number of stacking differences in crystals, and surface weak oxidation in (111)-oriented α-MnSe were the main mechanisms. Furthermore, α-MnSe nanosheets exhibited broadband photoresponse from 457 to 671 nm with an outstanding detectivity and responsivity behaviours. This study presents the detailed growth process of ultrathin 2D magnetic semiconductor α-MnSe, and its outstanding magnetic properties and broadband photodetection, which provide an excellent platform for magneto–optical and magneto–optoelectronic research.
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