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The discoveries of intrinsic ferromagnetism in atomically-thin van der Waalscrystals have opened up a new research field enabling fundamental studies onmagnetism at two-dimensional (2D) limit as well as development of magnetic vander Waals heterostructures. To date, a variety of 2D ferromagnetism has beenexplored mainly by mechanically exfoliating 'originally ferromagnetic (FM)' vander Waals crystals, while bottom-up approach by thin film growth technique hasdemonstrated emergent 2D ferromagnetism in a variety of 'originally non-FM' vander Waals materials. Here we demonstrate that V5Se8 epitaxial thin films grownby molecular-beam epitaxy (MBE) exhibit emergent 2D ferromagnetism withintrinsic spin polarization of the V 3d electrons despite that the bulkcounterpart is 'originally antiferromagnetic (AFM)'. Moreover,thickness-dependence measurements reveal that this newly-developed 2Dferromagnet could be classified as an itinerant 2D Heisenberg ferromagnet withweak magnetic anisotropy, broadening a lineup of 2D magnets to thosepotentially beneficial for future spintronics applications.

Intrinsic 2D Ferromagnetism in V5Se8 Epitaxial Thin Films